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Lasers and Co
11. Lasers and Coherent Light Sources

11.3 Semiconductor Lasers............................ 695


This chapter describes lasers and other sources

Part C 11
11.3.1 Overview .................................... 695
of coherent light that operate in a wide wave-
11.3.2 Resonator Types
length range. First, the general principles for
and Modern Active Layer Materials:
the generation of coherent continuous-wave and Quantum Effects and Strain .......... 698
pulsed radiation are treated including the inter- 11.3.3 Edge-Emitting Laser Diodes
action of radiation with matter, the properties with Horizontal Resonators .......... 703
of optical resonators and their modes as well 11.3.4 Basics of Surface-Emitting Lasers
as such processes as Q-switching and mode- with Vertical Resonators (VCSELs) ... 720
locking. The general introduction is followed by 11.3.5 Edge-Emitting Lasers and VCSELs
sections on numerous types of lasers, the em- with Low-Dimensional Active
phasis being on today’s most important sources Regions...................................... 725
of coherent light, in particular on solid-state 11.3.6 Lasers with External Resonators .... 725
lasers and several types of gas lasers. An im-
portant part of the chapter is devoted to the 11.4 The CO2 Laser........................................ 726
generation of coherent radiation by nonlin- 11.4.1 Physical Principles....................... 726
11.4.2 Typical Technical Designs.............. 737
ear processes with optical parametric oscillators,
difference- and sum-frequency generation, and 11.5 Ion Lasers ............................................ 746
high-order harmonics. Radiation in the extended 11.5.1 Ion-Laser Physics ........................ 747
ultraviolet (EUV) and X-ray ranges can be gener- 11.5.2 Plasma Tube Design..................... 749
ated by free electron lasers (FEL) and advanced 11.5.3 Ion-Laser Resonators................... 751
X-ray sources. Ultrahigh light intensities up to 11.5.4 Electronics.................................. 753
1021 W/cm2 open the door to studies of relativistic 11.5.5 Ion-Laser Applications ................. 755
laser–matter interaction and laser particle accel-
eration. The chapter closes with a section on laser 11.6 The HeNe Laser ..................................... 756
stabilization. 11.6.1 The Active Medium ...................... 756
11.6.2 Construction and Design Principles 758
11.6.3 Stabilization ............................... 762
11.6.4 Manufacturing ............................ 763
11.1 Principles of Lasers ............................... 584 11.6.5 Applications ............................... 764
11.1.1 General Principles ....................... 584
11.1.2 Interaction of Radiation 11.7 Ultraviolet Lasers:
with Atoms................................. 590 Excimers, Fluorine (F2 ), Nitrogen (N2 ) ...... 764
11.1.3 Laser Resonators and Modes ......... 595 11.7.1 The Unique Properties
11.1.4 Laser Rate Equations of Excimer Laser Radiation ........... 765
and Continuous-Wave Operation .. 602 11.7.2 Technology of Current Excimer Lasers
11.1.5 Pulsed Laser Behavior .................. 605 and the N2 Laser ......................... 765
11.7.3 Applications ............................... 770
11.2 Solid-State Lasers ................................. 614 11.7.4 Outlook: Radiation in the EUV ....... 775
11.2.1 Basics ........................................ 614
11.2.2 UV and Visible Rare-Earth Ion 11.8 Dye Lasers ............................................ 777
Lasers ........................................ 619 11.8.1 Overview .................................... 777
11.2.3 Near-Infrared Rare Earth Lasers .... 636 11.8.2 General Description ..................... 777
11.2.4 Mid-Infrared Lasers ..................... 660 11.8.3 Flashlamp-Pumped Dye Lasers ..... 777
11.2.5 Transition-Metal-Ion Lasers ......... 674 11.8.4 Tunable Dye Lasers Pumped by
11.2.6 Overview of the most Important High-Power Short-Wavelength
Laser Ions in Solid-State Lasers ..... 694 Lasers ........................................ 778
584 Part C Coherent and Incoherent Light Sources

11.8.5 Colliding-Pulse Mode-Locked 11.12 X-ray and EUV Sources........................... 819


Dye Lasers .................................. 778 11.12.1 X-Ray Lasers ............................... 819
11.8.6 Tunable Continuous-Wave 11.12.2 High-Order Harmonics ................. 822
Dye Lasers .................................. 779
11.8.7 Advanced Solid-State Dye Lasers ... 779 11.13 Generation of Ultrahigh Light Intensities
and Relativistic Laser–Matter Interaction 827
11.9 Optical Parametric Oscillators................. 785 11.13.1 Laser Systems for the Generation
11.9.1 Optical Parametric Generation ...... 786 of Ultrahigh Intensities ................ 827
Part C 11.1

11.9.2 Phase Matching .......................... 787 11.13.2 Relativistic Optics


11.9.3 Optical Parametric Oscillators ........ 790 and Laser Particle Acceleration...... 834
11.9.4 Design and Performance
of Optical Parametric Oscillators .... 790 11.14 Frequency Stabilization of Lasers ........... 841
11.10 Generation of Coherent Mid-Infrared Ra- 11.14.1 Characterization
diation by Difference-Frequency Mixing . 801 of Noise, Stability, Line Width,
11.10.1 Difference-Frequency Generation Reproducibility, and Uncertainty
(DFG) ......................................... 802 of the Laser Frequency ................. 842
11.10.2 DFG Laser Sources ........................ 809 11.14.2 Basics
11.10.3 Outlook ...................................... 813 of Laser Frequency Stabilization .... 845
11.14.3 Examples
11.11 Free-Electron Lasers ............................. 814 of Frequency-Stabilized Lasers...... 852
11.11.1 Principle of Operation .................. 814 11.14.4 Measurement
11.11.2 Current Status and Perspective of Optical Frequencies ................. 863
Applications of Free-Electron 11.14.5 Conclusion and Outlook ............... 864
Lasers ........................................ 815
11.11.3 Suggested further reading ............ 819 References .................................................. 864

11.1 Principles of Lasers


11.1.1 General Principles determined by the properties of its active medium. Alto-
gether, several thousand lasing lines have been reported
A laser (an acronym for light amplification by stim- ranging from the soft-X-ray down to the far-infrared
ulated emission of radiation) is a device that produces spectral region and new lines appear frequently in optics
and amplifies an intense beam of highly coherent, highly and laser journals. Depending upon the type of laser and
directional light. The original proposal of extending the its operational regime, the corresponding output power
maser (microwave amplification by stimulated emission may vary from a fraction of a milliwatt to several hun-
of radiation) idea to the infrared or visible region of dred kilowatts in continuous-wave operation, and from
the electromagnetic (EM) spectrum, thus giving a laser, tens of kilowatts to petawatt peak power in pulsed-mode
was however first made in 1960 by Maiman [11.1] us- operation.
ing a flash-pumped rod of ruby with polished ends A laser consists of at least three components
(ruby laser) after a proposal in 1958 by Townes and (Fig. 11.1):
Schawlow [11.2]. Nowadays laser devices range in size
1. a gain medium that can amplify light by means of
from semiconductor lasers as small as a grain of salt to
the basic process of stimulated emission;
solid-state lasers as large as a storage building. Lasers
2. a pump source, which creates a population inversion
are widely used in industry for, e.g., cutting and weld-
in the gain medium;
ing metals and other materials, in medicine for surgery,
3. two mirrors that form a resonator or optical cavity
in optical communications, in optical metrology, and
in which light is trapped, traveling back and forth
in scientific research. They are an integral part of such
between the mirrors.
familiar devices as bar-code scanners used in supermar-
kets, laser printers, compact disc and digital versatile The laser beam is usually the fractional part of light
disc (DVD) players. The output wavelength of a laser is trapped in the cavity that escapes from one of the two
Lasers and Coherent Light Sources 11.1 Principles of Lasers 585

R1 = 100 % R2 a) b) c)
l E2 2 E2 2 E2 2
2
Laser beam hí
Gain medium hí hí hí

1

Pumping E1 1 E1 1 E1 1

Part C 11.1
Mirror Output
mirror Fig. 11.2a–c Fundamental interaction processes of a quan-
tized atom with an EM wave. (a) Spontaneous emission.
Resonator
(b) Stimulated emission. (c) Absorption
Fig. 11.1 Schematic of a laser oscillator
the form of an EM wave, the process is referred to as
mirrors (the output coupler), which has a nonvanish- spontaneous, or radiative, emission (Fig. 11.2a). Owing
ing transmission at the laser oscillation wavelength. The to energy conservation, the frequency ν0 of the emitted
gain medium can be solid (including semiconductors), radiation is given by:
liquid, or gas, and the pump source can be an electrical (E 2 − E 1 )
discharge, a lamp, or another laser. Other specific com- ν0 = , (11.1)
h
ponents of a laser vary depending on the gain medium
and whether the laser is operated continuously or pulsed. where h is the Planck’s constant. Since the previous re-
Lasers may be in fact divided into two broad groups: lation can also be written as E 2 − E 1 = hν0 , we can say
that a single photon of energy hν0 is emitted during each
1. continuous wave (CW) or quasi-CW, spontaneous emission process. Note also that this pro-
2. pulsed. cess occurs even if the atom is isolated and no external
A CW laser exhibits a steady flow of coherent energy perturbation is applied. The probability of spontaneous
and its output power undergoes little or no change with emission can be characterized in the following way. Let
time. Many gas lasers, such as HeNe and Ar-ion lasers, us consider an ensemble of atoms and assume that, at
operate CW; several solid-state lasers, such as Nd3+ time t, there are N2 atoms per unit volume (population)
and Ti3+ :Al2 O3 lasers, are also often operated in CW in level 2.
mode. In pulsed lasers, the output beam power changes Quantum mechanical calculations show that the rate
with time so as to produce a short optical pulse, usu- of decay of these atoms due to spontaneous emission,
ally in a repetitive way and with pulse duration usually i. e., ( dN2 / dt)sp , is proportional to N2 according to:
ranging from nanoseconds (1 ns = 10−9 s) to femtosec-  
dN2 N2
onds (1 fs = 10−15 s). Typical examples of pulsed lasers =− , (11.2)
dt sp τs
are many solid-state and liquid lasers, such as Nd:YAG,
Ti:Al2 O3 , and dye lasers. where τs is referred to as the spontaneous emission life-
time and depends on the particular transition involved.
Spontaneous The direction, the polarization, and the phase of the
and Stimulated Emission, Absorption emission event are random, so that the overall emitted
A laser exploits three fundamental phenomena that occur light by the different atoms of the given population is
when an electromagnetic wave interacts with a mater- said to be incoherent.
ial, namely the processes of spontaneous and stimulated If the atom is not isolated but interacts, e.g., by col-
emission, and the process of absorption (Fig. 11.2). lisions with other atoms, the decay from the excited
state 2 to the ground state 1 may occur by a release
Spontaneous emission and nonradiative decay. Let of the internal energy (E 2 − E 1 ) into some form other
us consider the energy levels of some given material and than EM radiation (e.g., into kinetic or internal energy
indicate by E 1 and E 2 the energies of the ground level, of surrounding atoms in a gas or lattice vibrations in
1, and of an excited level, 2, of the medium. If the atom a crystal). The phenomenon is referred to as nonra-
is initially raised in the excited state 2, it spontaneously diative decay. The corresponding rate of decay from
tends to decay into the stable ground state 1. If the avail- the excited state 2 can usually be expressed in a sim-
able energy for the transition, E 2 − E 1 is released in ilar manner as (11.2), namely ( dN2 / dt)nr = −N2 /τnr ,
586 Part C Coherent and Incoherent Light Sources

where τnr is the nonradiative lifetime. When both radia- process of stimulated emission, the function σ21 (∆ν) is
tive and nonradiative decay are taken into account, the very narrow at around ∆ν = 0.
rate of decay of population N2 can be written as:
  Absorption. Lastly, let us consider the case of an atom
dN2 N2 N2 N2
=− − ≡− , (11.3) initially lying in its ground state 1. In the absence of
dt decay τs τnr τ perturbations, such as collisions with other atoms or with
where the time constant τ, defined by 1/τ = 1/τs + photons, the atom stably remains in this state. However,
Part C 11.1

1/τnr , is referred to as the lifetime of the excited state 2. if an EM radiation of frequency ν  ν0 is incident onto
the atom, there is a finite probability that the atom will be
Stimulated emission. If an EM wave of frequency ν raised to level 2. The energy difference E 2 − E 1 required
close to ν0 is incident onto the atom while in its excited by the atom to undergo the transition is obtained from
state 2, the interaction of the wave with the atom may the energy of the EM wave, namely one photon of the
stimulate the atom to decay to level 1 with the simultane- incoming wave is destroyed. This process is referred to
ous emission of EM radiation. The process is referred to as absorption (Fig. 11.2c). As for stimulated emission,
as stimulated emission. In this case, one photon, with the the absorption process can be described by
same frequency ν of the incoming radiation and with the  
dN2
same propagation direction, polarization state and phase = −W12 N2 , (11.5)
dt a
is emitted (Fig. 11.2b). This is a major distinction to
spontaneous emission. It is the fundamental reason why where W12 is the rate of absorption. Again one can show
a laser emits coherent light as compared to the incoher- that W12 = σ12 F, where σ12 is the absorption cross
ent light emitted by other light sources [such as lamps section. Einstein showed at the beginning of the 20th
or light-emitting diodes (LEDs)], which exploit sponta- century that, for nondegenerate levels, W12 = W21 , and
neous emission. Quantum mechanical calculations show thus σ12 = σ21 . If levels 1 and 2 are g1 -fold and g2 -fold
that the process of stimulated emission can be described degenerate, respectively, one then has g2 σ21 = g1 σ12 .
by the equation
  Coherent Amplification of Light
dN2
= −W21 N2 , (11.4) Consider a monochromatic EM plane wave at fre-
dt st quency ν which propagates along the z-direction inside
where W21 is the rate of stimulated emission. This rate is a medium made of a collection of atoms. Let E 1 and E 2
proportional to the photon flux F = I/(hν) of the incom- be the energies of two nondegenerate levels 1 and 2 of
ing wave, where I is the wave intensity. We can in fact the atom (this time 1 is not necessarily the ground state).
write W21 = σ21 F, where σ21 is a quantity having the We assume that the resonance frequency of the transi-
dimension of an area (the stimulated emission cross sec- tion, ν0 = (E 2 − E 1 )/h, is coincident (or very close) to
tion), which depends on the characteristics of the given ν. If F(z) is the photon flux of the EM wave at plane z
transition and on the frequency difference ∆ν = ν − ν0 , and N1 , N2 are the populations in levels 1 and 2 (which
i. e., σ21 = σ21 (∆ν). Owing to energy conservation in the are assumed to be z-independent), the change dF of the
photon flux due to the processes of absorption and stim-
ulated emission along the elemental length dz of the
a) b) material is given by (Fig. 11.3a)

óaa óa
S dF = σ(N2 − N1 )F(z) dz , (11.6)

F (z) F (z + dz)
óa óa
where σ ≡ σ21 = σ12 is the transition cross section. Note
óa that in writing (11.6) we did not consider radiative and
z óa
nonradiative decays since nonradiative decay does not
óa add new photons whereas spontaneous emission cre-
óa
ates photons which are emitted in any direction and
thus gives negligible contribution to the incoming pho-
dz
ton flux. Most importantly, note that for N2 > N1 , one
Fig. 11.3a,b Coherent amplification of an EM wave. (a) Photon has dF/ dz > 0 and the EM wave is amplified during
flux-balance diagram in an infinitesimal section dz of the amplifier. propagation, i. e., the medium acts as a coherent optical
(b) Physical meaning of the transition cross section amplifier. Conversely, for N2 < N1 , one has dF/ dz < 0
Lasers and Coherent Light Sources 11.1 Principles of Lasers 587

and the medium behaves as an absorber. If we let l be tical amplification instead of optical absorption, we need
the length of the medium, the photon flux F(l) at the out- to create population inversion in the medium by means
put plane is related to the one F(0) at the input plane by of a pumping process [11.3, 4], which drives the popu-
the relation F(l) = F(0) exp(g), where g = (N2 − N1 )σl lation distribution far from thermal equilibrium. At first
is the gain coefficient. The condition for light amplifica- sight one might think to achieve population inversion
tion (g > 0) is therefore N2 > N1 , which is often referred between levels 2 and 1 through the interaction of the
to as population inversion. We note that in the previous material with some strong EM radiation at frequency

Part C 11.1
calculation N1 and N2 have been assumed independent ν0 , such as that emitted by a flash or arc lamp. Since
of the intensity I of propagating wave. This is fine how- at thermal equilibrium N1e > N2e , absorption will domi-
ever provided that I is weak enough so as that changes nate over stimulated emission, and this will produce an
of N1 and N2 due to absorption and stimulated emis- increase of N2 and a decrease of N1 from their thermal
sions can be neglected; however, for strong intensities equilibrium values. However, when N1 tends to reach
one needs to account for the phenomenon of saturation. the same value of N2 , absorption and stimulated emis-
As a final comment, we note that an examination of sion processes compensate each other, i. e., the medium
(11.6) leads to a simple physical interpretation of the tends to become transparent. Such a situation is referred
transition cross section σ. First, let us suppose that all to as saturation of the two-level transition. Therefore,
the atoms of the medium are in the ground state and let owing to saturation, it is impossible to produce popu-
us associate with each atom an effective absorption cross lation inversion in a two-level system (at least in the
section σa in the sense that, if a photon enters this cross steady state). This goal can be achieved, however, when
section, it is absorbed by the atom (Fig. 11.3b). If S is more than two energy levels are considered. Typically
the cross-sectional area of the EM wave, the number of three or four energy levels are involved (Fig. 11.4), and
atoms in the element dz of the material is Nt S dz (Nt is correspondingly one speaks of three-level or four-level
the total atomic population, i. e., N1 = Nt and N2 = 0), lasers. In a three-level laser (Fig. 11.4a), atoms are raised
thus giving a total absorption cross section of σa Nt S dz. from the ground level 1 to the level 3 through a pump-
The fractional decrease of photon flux in the element dz ing mechanism. If the material is such that, once an
of the material is therefore ( dF/F) = −(σa Nt S dz/S) = atom excited into level 3 rapidly decays into a lower
−σa Nt dz. If we compare this expression with (11.6), level 2 (by, e.g., a fast nonradiative decay), then popu-
we conclude that σa = σ, so that the meaning we can lation inversion can be obtained between level 2 and 1.
attribute to σ is that of an effective absorption cross Note that, in a three-level laser scheme, to achieve pop-
section as just defined. ulation inversion it is necessary to raise at least half of
the atoms from the ground state 1 to state 3. In a four-
Population Inversion: The Pumping Process level laser (Fig. 11.4b), atoms are again raised from the
At thermal equilibrium any material behaves as an ab- ground level 0 to an excited state 3, with a rapid decay
sorber. In fact, the distribution of populations N2e and to the upper laser level 2; however this time laser ac-
N1e of levels 1 and 2 at thermal equilibrium is described tion takes place from level 2 to an excited lower-lying
by the Boltzmann statistics level 1. Once laser oscillation starts, level 1 is populated
  by stimulated emission; therefore to maintain popula-
N2e E2 − E1
= exp − , (11.7)
N1e kB T
where kB is the Boltzmann constant and T is the absolute a) b)
temperature. Note that N2e < N1e ; in particular N2e is neg- Pump level Pump level
3 3
ligible as compared to N1e if kB T  E 2 − E 1 ; at room Fast decay Fast decay
temperature (T = 300 K) one has kB T  208 cm−1 . 2 2
[A reciprocal centimeter is a simple convenient unit
Laser
for measuring energies in spectroscopy and refers to Laser
Pumping Pumping
the inverse of the wavelength of a photon possess- 1
ing the given energy E. The actual energy E in the Fast decay
SI unit (Joule) can be obtained by multiplying cm−1 1 0
Ground state Ground state
by hc, with c = 3 × 1010 cm/s and h = 6.63 × 10−34 Js].
Therefore the condition N2e  N1e is well satisfied for Fig. 11.4a,b Schematic of the energy-level diagram for (a) a three-
transitions in the near-infrared and visible. To obtain op- level laser, and (b) a four-level laser
588 Part C Coherent and Incoherent Light Sources

tion inversion in stationary conditions (continuous-wave by the active medium. Solid-state gain media, such as
operation), the lower laser level 1 should rapidly depop- Nd:YAG, and liquid lasers are particularly well suited
ulate through, e.g., a very fast nonradiative decay into to optical pumping: absorption lines are in fact very
the ground state 0. Compared to a three-level laser, the broad and this makes the absorption of the (broadband)
four-level laser offers the great advantage that population light of the lamps efficient. The flashlamps generate sig-
inversion is ideally achieved when just one atom is raised nificant heat into the material that must be dissipated
to the pumping level 3. Four-level lasers are thus more by water cooling. The pumping source may, however,
Part C 11.1

used, whenever possible, than three-level lasers. More itself be a laser; in this case one speaks of laser pump-
recently, the so-called quasi-three-level lasers have also ing. Among the most used laser pump sources, we just
become a rather important laser category. In these lasers mention semiconductor lasers (diode laser pumping),
the energy level scheme is similar to that of a four-level argon-ion laser and second-harmonic or third-harmonic
laser, however levels 0 and 1 are now nondegenerate generation of Nd lasers. With the advent of powerful
sublevels of the ground energy level. The population of and reliable semiconductor lasers, diode-laser pumping
the ground state is distributed in all the sublevels ac- is nowadays commonplace for many solid-state and fiber
cording to Boltzmann statistics, and therefore, at room lasers.
temperature, some population is left in level 1.
The mechanism that allows atom excitation from the Electrical pumping. In gas lasers and semiconductor
ground energy level into the excited pump level 3 is re- lasers, the excitation mechanism usually consists of
ferred to as the pumping process. The rate of population an electrical current flow through the active medium.
of the upper state, 2, due to the pumping, ( dN2 / dt)p , Gas lasers generally need to be electrically pumped be-
can be written as: cause, due to the small width of their absorption lines,
  optical pumping would be very inefficient. In gas lasers,
dN2
= Wp Ng , (11.8) electrical pumping is achieved by passing an electric
dt p
current either CW, at radio frequency or pulsed, directly
where Wp is the pumping rate and Ng is the popula- through the gas itself. During the discharge, ions and
tion of the ground state. For a four-level laser, one can free electrons are produced which acquire kinetic en-
assume Ng to be constant (and much larger than N2 ). ergy from the applied field and are able to excite neutral
In this case one can write from (11.8) ( dN2 / dt)p = Rp , atoms via collisions: A + e → A∗ + e, where A∗ denotes
where Rp = Wp Ng is the pump rate per unit volume. The the atomic species in an excited state. Since electron im-
energy required for pumping is generally supplied either pact excitation is a nonresonant process, it is a rather
optically or electrically. The minimum pump power Pm efficient pumping method for a gas. In some cases, the
needed to produce a given pump rate Rp is given by gas may contain two species, one of which is first excited
Pm = ( dN2 / dt)p Vhνmp , where ( dN2 / dt)p is the num- by the discharge and then undergoes resonant energy
ber of atoms per unit volume and time raised to the upper transfer with the other via collision (an example is the
laser level by the pumping process, V is the volume of HeNe laser). Electrical pumping in semiconductor lasers
the active medium, and νmp is the minimum pump fre- is achieved by flowing a large current density in a p–n
quency, given by the difference between the ground level or p–i–n diode. Though optical pumping can be used for
and the upper laser level. For either electrical or opti- semiconductor lasers, electrical pumping proves to be
cal pumping, the actual pump power Pp turns out to be much more convenient.
larger than the minimum value Pm , so that one can define Pumping processes different from optical or elec-
a pump efficiency ηp = Pm /Pp . Therefore, the relation trical pumping may also be employed in some special
between the pump rate Rp and the actual pump power lasers; we just mention chemical pumping in chemical
Pp is given by: lasers, where population inversion is produced directly
  from an exothermic reaction.
Pp
Rp = ηp . (11.9)
Vhνmp Laser Oscillation
To obtain laser oscillation, the amplifying medium is
Optical pumping. In optical pumping by an incoherent placed between two mirrors, forming a laser cavity
source, light from a powerful lamp (usually medium- to (Fig. 11.1). Light propagating along the cavity axis and
high-pressure Xe and Kr flashlamps for pulsed lasers, passing through the pumped laser medium is reflected
or high-pressure Kr lamps for CW lasers) is absorbed back through it, stimulating further emission in the same
Lasers and Coherent Light Sources 11.1 Principles of Lasers 589

direction. This means that laser photons undergo mul- be calculated from a balance between the number of
tiple reflections within the cavity, being amplified at atoms pumped per unit volume and time in the upper
each pass through the laser medium. One mirror (to- laser level and the number of atoms that decay via ra-
tal reflector) reflects almost all the incident light back diative and nonradiative ways. Assuming N1  0, one
through the laser medium while the other (partial reflec- obtains ∆N  N2 = Rp τ. When N2 = Nc , from the pre-
tor or output coupler) transmits a fraction T2 = 1 − R2 , vious equation and with the help of (11.10) the critical
which constitutes the output laser beam. The combina- pump rate is obtained as Rcp = γ /(στl). Note that the

Part C 11.1
tion of laser gain medium, pumping source and optical critical pump rate increases as στ decreases. Therefore
cavity forms a simple laser oscillator: if the amplifi- the product στ, which depends on the properties of the
cation is large enough to overcame losses, i. e., when given transition, can be regarded as a figure of merit for
a threshold condition is reached, a single photon (which a given laser.
is always present due to quantum noise) can be ampli-
fied by several orders of magnitude to produce a huge Properties of Laser Beams
number of coherently generated photons trapped inside Laser radiation shows an extremely high degree
the resonator. In addition, for an open resonator, only the of monochromaticity, coherence, directionality and
photons which propagate in the paraxial direction of the brightness as compared to other noncoherent light
resonator axis can reach the threshold for oscillation, so sources [11.3].
that an important property of the output laser beam is that The monochromaticity of laser radiation results from
it is directional. We can obtain the threshold condition the circumstance that light oscillation sets in at one res-
for laser action by a simple argument based on gain/loss onance frequency of the optical cavity, and owing to the
balance of light photons in one cavity round-trip. In balance between gain and loss in CW operation the line
fact, in one round-trip the photons pass twice through width ∆νL of the oscillating mode is ultimately limited
the gain medium and hence the round-trip gain of pho- by quantum noise. Conversely, light from incoherent
tons is exp(2σ Nl), where N = N2 − N1 is the population sources which exploit spontaneous emission (including
inversion, and l is the length of the active medium. On LEDs) has a much lower degree of monochromaticity (as
the other hand, the round-trip loss for photons can be much as 11 orders of magnitude) since the spectral distri-
written as (1 − T1 )(1 − T2 )(1 − L i )2 , where T1 = 1 − R1 bution of spontaneously emitted photons is broadened at
and T2 = 1 − R2 are the power transmission of the two around the atomic resonance frequency ν0 owing to var-
mirrors whereas L i accounts for the one-way internal ious broadening mechanisms. For laser radiation in the
loss in the cavity (due to, e.g., scattering or diffraction visible or near-infrared, line widths ∆νL as low as a few
loss for open resonators). The population inversion Nc Hz may, in fact, be achieved in frequency-stabilized laser
needed to reach threshold (also called critical inversion) sources.
is simply obtained by equating the round-trip gain and The coherence of laser radiation refers to either tem-
loss. After setting γ1 = −ln(1 − T1 ), γ2 = −ln(1 − T2 ) poral or spatial coherence. To define spatial coherence,
and γi = −ln(1 − L i ), the critical inversion turns out to let us consider two points P1 and P2 that, at a time t = 0,
be given by belong to the same wavefront, i. e., the phase difference
γ between their electric fields at time t = 0 is zero. If the
Nc = , (11.10) difference ϕ2 (t) − ϕ1 (t) of their phases also remains zero
σl at times t > 0, we say that there is perfect spatial coher-
where ence between the two points P1 and P2 . In practice, for
γ1 + γ2 any point P1 , in order to have some degree of phase cor-
γ = γi + (11.11) relation, point P2 must lie within some finite area around
2 P1 , which is called the coherence area. The high degree
is referred to as the single-pass logarithmic loss of the of spatial coherence of laser radiation stems again from
cavity. Once the critical inversion is reached, oscillation the fact that the spatial field distribution of the beam gen-
builds up from spontaneous emission. erated by stimulated emission is a mode of the optical
To calculate the pump rate Rcp needed to reach the resonator.
threshold condition (the critical pump rate), let us con- To define temporal coherence at a given point P, let
sider the four-level laser (Fig. 11.4b). In steady-state us consider the phase difference ϕ(t + τ) − ϕ(t) for the
conditions and in the absence of lasing, the popula- electric field at P at times t + τ and t. For a given de-
tion accumulated on the upper laser level can simply lay τ, if the phase difference is independent of time t,
590 Part C Coherent and Incoherent Light Sources

we say that there is temporal coherence over a time τ. 11.1.2 Interaction of Radiation with Atoms
If this occurs for any value of τ, the EM wave is said
to have perfect temporal coherence. If, conversely, this Absorption and Stimulated Emission Rates
occurs only for delays τ smaller than a given delay τ0 , Consider a monochromatic EM wave of frequency ν in-
the wave is said to have partial temporal coherence, cident on a two-level atom with a transition frequency
and τ0 is called the coherence time of the EM wave at ν0 = (E 2 − E 1 )/h close to ν. The calculation of the ab-
point P. The concept of temporal coherence is closely sorption and stimulated emission rates W12 and W21 can
Part C 11.1

related to that of monochromaticity; in fact, for a CW be done following a semiclassical approach, in which
laser one can show that the coherence time τ0 is re- the atom is treated quantum mechanically whereas the
lated to the laser line width ∆νL by the simple relation EM wave classically [11.3,5–9]. If the atom is initially in
τ0 ≈ 1/∆νL . The high degree of temporal coherence of its ground state (level 1), the incident wave may induce
laser radiation is therefore due to its extreme degree of a transition to level 2 owing to the coupling of the elec-
monochromaticity. tromagnetic field with the electric and magnetic dipole
The directionality of the laser beam is due to the fact (and multipole) moments of the atom. The strongest in-
that the gain medium is placed inside an open optical teraction is usually that arising between the electric field
resonator and, as a consequence, stimulated emission E(t) = E0 cos(2πνt) of the EM and the electric dipole
preferentially occurs in the direction orthogonal to the moment of the transition, which is defined by the ma-
two cavity mirrors (Fig. 11.1), where feedback from the trix dipole element µ12 = u ∗2 (r)eru 1 (r) dr, where r is
mirrors is most effective and diffraction losses are the the distance of the electron of the atom, with charge
smallest. The laser beam emitted from the output cou- e, from its nucleus, and where u 1 (r) and u 2 (r) are the
pler shows a divergence angle which, in the ideal case, is electronic eigenfunctions for the atomic energy levels 1
limited by diffraction. From diffraction theory, the diver- and 2 respectively. In this electric-dipole approximation,
gence angle for a monochromatic beam of wavelength a perturbation theory, which assumes that the interaction
λ turns out to be given by between the EM wave and the atom is not disturbed by,
  e.g., collisions or other phenomena (including sponta-
λ
θd = β , (11.12) neous emission), leads to the following expression for
2w the absorption and stimulated emission rate
where β is a numerical coefficient (of order 1) whose 2π 2
specific value depends on the particular transverse field W12 = W21 = |µ12 |2 ρδ(ν − ν0 ) , (11.14)
3n 2 0 h 2
distribution and 2w is the diameter of the beam. For
example, considering laser radiation in the visible (λ = where ρ = n 2 0 E 02 /2 is the energy density of the EM
500 nm), the divergence of a laser beam of transverse wave, n is the refractive index of the medium, and δ is the
diameter 2w ≈ 1 cm is solely θd ≈ λ/2w  5 × 10−5 rad. impulse Dirac function. In particular, for a plane wave
This means that, after propagation for a length L = 1 km, of intensity I = cρ/n, from (11.14) the following ex-
the beam size is increased to solely w + θd L ≈ 6 cm! pression for the cross section σ12 = W12 /F = hνW12 /I
The brightness of laser radiation is closely related to can be derived:
the directionality and stems from the capability of a laser 2π 2
oscillator to emit a high optical power in a small solid σ12 = |µ12 |2 νδ(ν − ν0 ) . (11.15)
3n 0 ch
angle of space. For a given emitting source, of area ∆S,
if P denotes the optical power delivered in a fractional Analogously, if initially the electron is on level 2, owing
solid angle ∆Ω of space, the brightness of the emitter to the interaction with the EM wave there is a prob-
is defined as B = P/(∆S∆Ω). The brightness of a laser ability that the electron decays into state 1 emitting
source, in which the solid angle of emission ∆Ω is a photon by stimulated emission. The semiclassical per-
determined by its divergence angle θd , is given by turbation calculation leads for the stimulated emission
cross section σ21 = hνW21 /I the same expression as that
  of σ12 , i. e., σ21 = σ12 , provided that the two levels are
2 2
B= P. (11.13) not degenerate.
βπλ
The expression for σ12 = σ21 as given by (11.15) is
A laser of moderate power (e.g., a few milliwatts) has unphysical since it implies that the transition probability
a brightness several orders of magnitude greater than is zero for ν = ν0 and ∞ for ν = ν0 . The inconsis-
that of the brightest conventional sources. tency is removed by observing that the interaction of
Lasers and Coherent Light Sources 11.1 Principles of Lasers 591

the monochromatic EM wave with the atom is not per-


fectly coherent, but it is disturbed by, e.g., collisions a) g b) g*
0.939
with other atoms or with lattice phonons, spontaneous Äí*0
emission and nonradiative decay of the atom. The effect 0.637
of such disturbing interactions is to broaden the tran- Äí0
sition line of each atom in the ensemble, in the sense
Äí*0
that in (11.15) the Dirac δ function δ(ν − ν0 ) should be Äí0

Part C 11.1
replaced by a new function g(ν − ν0 ), symmetric about
ν = ν0 with g(ν − ν0 )dν = 1, which is generally given 0 í – í0 0 í– í0
by the Lorentzian function (Fig. 11.5a):
Fig. 11.5 Lorentzian (left side) and Gaussian (right side) line
2 1 shapes corresponding to homogeneous and inhomogeneous tran-
g(ν − ν0 ) = , (11.16)
π∆ν0 1 + [2(ν − ν0 )/∆ν0 ]2 sition broadening, respectively

where ∆ν0 depends on the particular broadening mecha- assumes the most general form:
nism involved. Note that the full width at half-maximum
(FWHM) of the Lorentzian function is simply ∆ν0 . 2π 2
σ= |µ12 |2 νgt (ν − ν0 ) , (11.18)
The resonant character of the stimulated emission and 3n 0 ch
absorption processes is maintained since the line broad- where the total line shape gt is given by the convolution:
ening ∆ν0 is typically several orders of magnitude 
smaller than ν0 (e.g., in a low-pressure gas, for a tran- gt (ν − ν0 ) = g∗ (ν0 − ν0 )g(ν − ν0 ) dν0 . (11.19)
sition in the visible one has ν0 ≈ 5 × 1014 Hz whereas
∆ν0 ≈ 106 –108 Hz). Since the aforementioned broad- If we consider an ensemble of atoms and indicate by
ening mechanism act in the same way on each atom N1 and N2 the populations of atoms in the energy
of the ensemble, it is referred to as a homogeneous levels 1 and 2, as discussed in the previous section
broadening mechanism. a small-signal EM wave of frequency ν which prop-
A somewhat different case occurs when the reso- agates inside the medium experiences amplification
nance frequencies ν0 of the atoms in the ensemble are for N2 > N1 or absorption for N2 < N1 . In the for-
distributed around a central frequency ν0 (inhomoge- mer case, one can introduce the absorption coefficient
neous broadening). This distribution
 is described by the per unit length α(ν) = σ(ν − ν0 )(N1 − N2 ), whereas
function g∗ (ν0 − ν0 ) such that g∗ (ν0 − ν0 ) dν0 = 1 and in the latter case one can introduce the gain coeffi-
g∗ (ν0 − ν0 ) dν0 is the fractional part of the atoms in the cient per unit length g(ν) = σ(ν − ν0 )(N2 − N1 ). For
ensemble whose resonance frequency lies in the inter- a weak-signal wave, so that saturation can be ne-
val (ν0 , ν0 + dν0 ). For the most common mechanisms glected, the intensity of the propagating wave is thus
of inhomogeneous line broadening (such as Doppler exponentially attenuated or amplified along the propa-
broadening in a gas or local-field effects in ionic crys- gation direction according to I(z) = I(0) exp(−αz) or
tals or glasses) the distribution g∗ (ν0 − ν0 ) is given by I(z) = I(0) exp(gz), respectively.
a Gaussian function (Fig. 11.5b): These considerations apply to atomic or molecu-
  lar transitions which are electric-dipole allowed, i. e.,
2 ln2 1/2 for which the dipole matrix element µ12 of the tran-
g∗ (ν0 − ν0 ) =
∆ν0∗ π sition does not vanish. Transitions between atomic or
  molecular energy levels with the same parity (e.g., be-
4ln2(ν0 − ν0 )2 tween s states in an atom) are electric-dipole forbidden.
× exp − , (11.17)
∆ν0∗2 This does not mean however that the atom or molecule
cannot pass from level 1 to level 2 when interacting
where ∆ν0∗ is the transition line width (FWHM), which with an EM wave; in this case the transition can oc-
depends on the particular broadening mechanism. cur owing to the interaction of the EM wave with, e.g.,
Taking into account the simultaneous presence the magnetic dipole moment (or the electric quadrupole
of both homogeneous and inhomogeneous broaden- moment) of the transition, though the strength of the
ing mechanisms, one can show that the cross section cross section describing this process is much smaller
σ = σ12 = σ21 for stimulated emission and absorption than that of an allowed electric dipole transition. For an
592 Part C Coherent and Incoherent Light Sources

electric dipole transition the absorption transition rate where ρ(ν) is such that ρ(ν) dν is the EM energy per
W e is proportional to ∼ |µ e E 0 |2 , where µ e is the elec- unit volume of the cavity associated to modes with fre-
tric dipole moment of the transition, E 0 the amplitude of quencies in the interval (ν, ν + dν). We note that in
the electric field of the EM wave and −E 0 µ e is the clas- (11.21) the factor (8πν2 /c3 ) represents the density of
sical energy of an electric dipole in an external field E 0 . EM modes per unit volume of the cavity, whereas the
Likewise, for a magnetic dipole interaction, the transi- term hν/[exp(hν/kB T ) − 1] is the energy per mode. The
tion rate Wm is proportional to ∼ |µm B0 |2 , where µm populations N1e and N2e in the atomic levels 1 and 2 at
Part C 11.1

is the magnetic dipole of the transition, B0 is the ampli- thermal equilibrium are described by a Boltzmann statis-
tude of the magnetic field of the EM wave, and −B0 µm tics (11.7); on the other hand, at steady state the number
is the classical energy of a magnetic dipole in an exter- of excitation per unit time from level 1 to level 2 due
nal magnetic field B0 . By approximating µ e ≈ ea and to the absorption of black-body radiation should bal-
µm ≈ β, where a = 0.529 × 10−10 m is the Bohr radius ance the number of decays per unit time from level 2 to
and β = 9.27 × 10−24 Am2 is the Bohr magneton, one level 1 due to both stimulated emission and spontaneous
then obtains: emission, i. e., W12 N1e = W21 N2e + N2e /τs . One then
      obtains 1/τs = W12 exp(hν0 /kT ) − W21 . For a spec-
We eaE 0 2 eac 2
= =  105 . (11.20) trally broad radiation (such as  black-body radiation)
Wm β B0 β one can write W12 = W21 = dνcσ(ν − ν0 )ρ(ν)/nhν
= 2π 2 |µ12 |2 ρ(ν0 )/(3n 2 0 h 2 ), where we used (11.15).
Spontaneous Emission Using this expression for W12 = W21 and (11.21) for
Spontaneous emission is the phenomenon by which ρ(ν0 ), one finally obtains
an atom in an excited energy level tends to decay to- 3h 0 c3
ward the ground state (even in absence of any external τs = . (11.22)
perturbation) by emitting an EM wave, i. e., one photon. 16π 3 ν03 n|µ12 |2
A correct explanation of spontaneous emission requires Using a similar thermodynamic argument, one can also
a quantum electrodynamic approach in which both the show that the spectrum of the photon emitted by spon-
atom and the EM field are quantized. In practice, due to taneous emission is given by the line shape gt (ν − ν0 ) of
quantization of the EM field, the mean values of both the transition (11.19), i. e., the probability that the pho-
E 2 and H 2 fields are nonvanishing even in the absence ton emitted by spontaneous emission has a frequency in
of a (classical) EM wave (zero-point field fluctuations). the range (ν, ν + dν) is given by gt (ν − ν0 ) dν. This prop-
Such intrinsic fluctuations always perturb the atom in an erty is very interesting since it enables one to measure
excited state and trigger its decay toward a lower energy the transition line shape gt (ν − ν0 ) simply in an emission
level with the emission of one photon with frequency experiment by passing the spontaneously emitted light
ν close to the atomic transition frequency ν0 . Atomic through a spectrometer of sufficiently high resolution.
decay due to spontaneous emission follows an exponen- To estimate the radiative lifetime τs , let us con-
tial law with a time constant τs , which is referred to sider for instance an electric-dipole-allowed transition
as the spontaneous emission lifetime [see (11.2)]. The at a frequency corresponding to the middle of the visi-
quantum electrodynamic calculation of τs in the electric ble range (λ0 = c/ν0 = 500 nm). Assuming |µ12 |  ea
dipole approximation and for an atom placed in an op- (where a  0.1 nm is the atomic radius), from (11.22)
tical cavity was done by Weisskopf and Wigner [11.10]. one obtains τs  10 ns. For a magnetic dipole transition
A simple and rigorous calculation of τs may be derived 1/τs turns out to be 105 times smaller, i. e., τs  1 ms.
using an elegant thermodynamic argument, which was Note that, according to (11.22), τs decreases as the cube
proposed by Einstein well before any development of the of the transition frequency, so that the importance of
quantum electrodynamics [11.11]. Assume that the ma- spontaneous emission increases rapidly with frequency.
terial is placed inside a black-body cavity whose walls This implies that, as spontaneous emission is often neg-
are kept at a constant temperature T . Once the thermo- ligible in the middle- to far-infrared, where nonradiative
dynamic equilibrium is reached, the spectral EM energy decay dominates, in the X-ray region (e.g., λ0 < 5 nm)
density distribution ρ(ν) inside the cavity is given by the spontaneous emission is the dominant decay process
Planck distribution and τs becomes exceedingly short (10–100 fs). Such
  a short lifetime represents a major challenge for achiev-
8πν2 hν
ρ(ν) = (11.21) ing a population inversion in X-ray lasers. It should
c3 exp(hν/kT ) − 1 finally be noted that the rate of spontaneous emission as
Lasers and Coherent Light Sources 11.1 Principles of Lasers 593

given by (11.22) can be either enhanced or reduced when


the atom radiates in a dielectric cavity whose density of 1
EM modes (i. e., the number of resonant cavity modes í
per unit frequency and per unit volume) is changed from
the value (8πν2 /c3 ) due to, e.g., tight spatial confine-
ment, such as in microlasers. For instance, spontaneous t
decay is fully inhibited for an atom placed inside a pho-

Part C 11.1
tonic crystal whenever the atomic transition frequency
ν0 falls inside a bandgap of the photonic crystal. ô

Line Broadening Mechanisms Fig. 11.6 Schematic of the sinusoidal electric field of fre-
Homogeneous broadening. A line broadening mech- quency ν showing random phase jumps at time intervals τ
anism is said to be homogeneous when it broadens the
line of each atom in the same way. In this case the line by W12 = σ12 (ν − ν0 )I/hν, where the cross section σ12
shape of the single-atom cross section and that of the is given by (11.15) after replacing the delta function
overall absorption cross section are identical. There are δ(ν − ν0 ) with g(ν − ν0 ). To calculate the line shape g,
two main homogeneous broadening mechanisms: colli- let us assume that the distribution of the time interval τ
sional broadening and natural broadening. between two successive collisions be described by an ex-
Collisional broadening occurs in a gas, where the ponential probability density, p(τ) = [exp(−τ/τc )]/τc ,
atom may collide with other atoms, ions, free elec- where τc is the mean value of τ. According to the
trons, or with the walls of the container, as well as in Wiener–Kintchine theorem, the spectrum g can be cal-
a solid, where collisions are due to the interaction of culated as the Fourier transform of the autocorrelation
the atom with the lattice phonons. During a process of function of the sinusoidal field with phase jumps at
absorption or stimulated emission of a two-level atom time intervals τ (Fig. 11.6). This yields a Lorentzian
with a monochromatic EM wave, the collisions inter- line shape (11.16) with a FWHM of ∆ν0 , related to the
rupt the coherent interaction of the EM with the atom; mean value of collision time τc by the equation
if we write the electronic wave function ψ of the atom 1
during the transition as ψ = c1 (t)u 1 (r) exp[−iE 1 t/ ] + ∆ν0 = . (11.23)
c2 (t)u 2 (r) exp[−iE 2 t/ ], assuming that the collision πτc
does not induce a decay, it simply introduces a ran- For instance, for an atomic or molecular gas at pres-
dom and rather instantaneous relative phase jump of the sure p and absolute temperature T , from kinetic theory
coefficients c1 and c2 , and
 thus of the oscillating part of and employing the hard-sphere model of a gas, one has
the atomic dipole µ = −er|ψ(r, t)|2 dr, which is pro- τc = (2MkB T/3)1/2 [1/(8π pa2 )], where M is the atomic
portional to c1 c∗2 . Since in the electric-dipole interaction mass and a its radius. Note that τc is inversely propor-
the radiation–atom coupling is expressed by the energy tional, and hence ∆ν0 is directly proportional, to the gas
term −µ e E, a different but equivalent picture is to as- pressure p. As a rough rule of thumb, we can say that,
sume that it is the phase of the electric field that shows for any atom in a gas, collisions contribute to the line
random phase jumps rather than the atomic dipole mo- broadening by an amount (∆νcoll / p) ≈ 1 MHz/Torr.
ment (Fig. 11.6). Therefore we can consider the case of For an atom or an ion in a crystal, collisions occur
coherent (i. e., not disturbed) interaction of the two-level with lattice phonons. Since the number of phonons in
atom with an EM wave which is not monochromatic but a given lattice vibration is strongly dependent on the
whose spectral content is broadened at around ν owing lattice temperature T , the corresponding line broad-
to the phase jumps. Let I(ν ) = Ig(ν − ν) be the spec- ening ∆ν0 increases with increasing values of T . For
tral intensity distribution of the EM wave with random instance, in the Nd:YAG laser Nd3+ ions are hosted
phase jumps (Fig. 11.6), where I is the total field inten- in the YAG crystal, and collision broadening increases
sity and g its spectral shape (with g(ν − ν) dν = 1). from ∆ν0 ≈ 126 GHz at room temperature (T = 300 K)
For each fractional spectral component Ig(ν − ν) dν of to about 250 GHz at T = 400 K.
the EM wave, we may introduce an elemental absorp- A second homogeneous line broadening mechanism
tion transition rate dW12 given, according to (11.14), by originates from spontaneous emission and is referred
dW12 = [2π 2 |µ12 |2 /(3n 0 ch 2 )]δ(ν
 − ν0 )Ig(ν − ν) dν . to as natural (or intrinsic) line broadening. It can be
The total transition rate, W12 = dW12 , is then given shown that the natural broadening is again described by
594 Part C Coherent and Incoherent Light Sources

a Lorentzian function with a FWHM of ∆ν0 given by the HeNe laser, at T = 300 K and using the appropriate
1 mass for Ne, one obtains ∆ν0∗  1.7 GHz. As a general
∆ν0 = , (11.24) rule, Doppler broadening in a gas is usually larger than
2πτs
collisional broadening for a gas pressure lower than the
where τs is the spontaneous lifetime. For, e.g., an atmospheric pressure; collisional broadening, in turn, is
electric dipole transition at the center of the vis- usually larger than the natural broadening.
ible (λ ≈ 500 nm), one has ∆νnat  16 MHz. Since
Part C 11.1

τs ≈ 1/ν3 , the natural line width rapidly increases for Nonradiative Decay
transitions at shorter wavelengths (to the UV or X-ray Besides decaying via radiative emission, an atom in an
spectral regions). excited state may decay toward a lower-lying level in
We finally note that, when the two aforementioned a nonradiative way. A first mechanism of nonradiative
homogeneous line broadening mechanisms act simul- decay arises from collisions and is called collisional de-
taneously, the overall line shape is obtained from the activation. In this case, for a liquid or a gas, the transition
convolution of the two corresponding Lorentzian func- energy is released as excitation and/or kinetic energy
tions. One then obtains a Lorentzian function with of the colliding species, or it is transferred to the con-
a FWHM given by ∆ν0 = ∆νcoll + ∆νnat . tainer walls; for an ion in a crystal or in a glass the
deactivation occurs through the interaction with lattice
Inhomogeneous broadening. A line broadening mech- phonons or glass vibrational modes. When, e.g., the ex-
anism is said to be inhomogeneous when it distributes citation energy of an atomic excited species B ∗ in a gas
the atomic resonance frequencies over some spectral is released as a kinetic energy of the species A, the col-
range. A first case of inhomogeneous broadening is that lisional deactivation process occurs via the superelastic
of ions in ionic crystals or glasses, where the local crys- collision B ∗ + A → B + A + ∆E, where ∆E, the exci-
tal field induces, via the Stark effect, a local variation of tation energy to be released, is left as kinetic energy of
the energy-level separation of the ion. For random lo- the colliding partners. When the electronic energy of
cal field variations, the corresponding distribution of the species B ∗ is released in the form of the internal energy
transition frequencies g∗ (ν − ν0 ) turns out to be given by of species A, we have instead B ∗ + A → B + A∗ + ∆E,
a Gaussian function (11.17) with a line width ∆ν0∗ that where now ∆E is the difference between the internal
depends on the amount of field inhomogeneity within energies of the two colliding species. In this latter case,
the crystal or glass. deactivation process is efficient provided that ∆E is
A second inhomogeneous mechanism, typical of appreciably smaller than the thermal energy kB T of col-
gases, arises from atomic motion and is referred to as liding species. A simple description of the nonradiative
Doppler broadening. In fact, due to the motion of the decay of a given species in an excited state is expressed
atom, the frequency ν of the EM wave as seen in the by a nonradiative lifetime τnr such that N2 /τnr is the
rest frame of the atom is shifted as compared to the fre- number of atoms, per unit volume and time, that decay
quency ν of the wave in the laboratory reference frame owing to the deactivation process.
according to the relation ν = ν[1 − (vz /c)], where vz Nonradiative decay acts in combination with spon-
is the component of the atomic velocity in the propa- taneous emission and, according to (11.3), the overall
gation z-direction of the EM wave. From the point of lifetime τ of an excited state is given by: τ = (1/τnr +
view of atom–radiation interaction, this shift is equiva- 1/τs )−1 .
lent to a change of the resonance frequency of the atom
rather than to a change of the EM frequency. Taking into Concluding Remarks
account the Maxwellian distribution of molecular ve- From the preceding discussions, we can say that the most
locities in a gas, one can show that the distribution of important material parameters of interest for a laser are
the transition frequencies g∗ (ν − ν0 ) is given again by the transition wavelength λ, the transition cross sec-
a Gaussian function (11.17) with a line width ∆ν0∗ given tion at the peak σp , the lifetime of the upper laser level
by τ, and the line width ∆ν0 of the transition line shape.
  These parameters, for the most common gas, liquid and
2kB T ln 2 1/2
∆ν0∗ = 2ν0 , (11.25) solid-state lasers, are summarized in Table 11.1. We
Mc2 note that, as compared to gas and liquid lasers, the cross
where M is the atomic (or molecular) mass and T the gas sections for solid-state lasers (Nd:YAG, Nd:glass, and
temperature. As an example, for the λ = 632.8 nm line of Ti3+ :Al2 O3 ) are relatively small and, correspondingly,
Lasers and Coherent Light Sources 11.1 Principles of Lasers 595

Table 11.1 Main parameters for transitions in most common gas, liquid and solid-state lasers
Transition λ (nm) σp (cm2 ) τ (µs) ∆ν0
HeNe 632.8 5.8 × 10−13 30 × 10−3 1.7 GHz
Ar+ 514.5 2.5 × 10−13 6 × 10−3 3.5 GHz
Nd:YAG 1064 2.8 × 10−19 230 120 GHz
Nd:glass 1054 4 × 10−20 300 5.4 THz
3.2 × 10−16 5.5 × 10−3

Part C 11.1
Rhodamine 6 G 570 46 THz
Ti3+ :Al2 O3 790 4 × 10−19 3.9 100 THz

the lifetimes relatively long because in these lasers the under the gainline of the HeNe laser is N ≈ 1.2 × 109 .
transitions are electric-dipole forbidden (or weakly al- In the open optical resonant cavities only those modes
lowed). We note also that the line widths of gas lasers traveling nearly parallel to the resonator axis experience
are much smaller than those of solid-state or dye lasers. low losses to allow for laser oscillation. Therefore, the
oscillating modes are expected to show a field distri-
11.1.3 Laser Resonators and Modes bution mostly confined around the optical axis of the
resonator and propagating paraxially along it, making
As discussed in the introductory section, in a laser os- the output laser beam highly directional. These cavity
cillator the inverted amplifying medium is placed inside modes and corresponding resonance frequencies depend
a laser resonator or laser cavity, which can be viewed upon three integer numbers n, m and l, which are re-
as a trapping box for light radiation capable of sustain- ferred to as mode indices. The latter two indices m and l
ing stationary (i. e., monochromatic) or weakly damped (transverse mode indices) determine the transverse field
electromagnetic field configurations at some selected distribution (i. e., in a plane orthogonal to the paraxial
optical frequencies [11.3, 5]. Such EM field configu- resonator axis) of the mode, whereas the former index
rations and the corresponding optical frequencies are n (the longitudinal mode index) determines the longitu-
called cavity modes and resonance frequencies, respec- dinal field distribution (i. e., along the resonator axis) of
tively. The most widely used resonators for lasers are the mode and gives, in particular, the number of longitu-
open cavities, composed of at least by two plane or spher- dinal nodes of the standing wave. For spherical mirrors
ical mirrors of circular shape (spherical resonators), with sufficiently wide apertures, transverse modes are
placed in front each other at some distance L. Ex- expressed by Gauss–Hermite or Gauss–Laguerre func-
cept for microlasers, in ordinary lasers the resonator tions, depending on rectangular or circular boundary
length L is typically much larger than the oscillat- conditions. In particular, the leading-order mode, cor-
ing wavelength λ, ranging from a few centimeters to responding to transverse mode indices m = l = 0, is
a few tens of centimeters, whereas mirror dimensions a Gaussian beam and represents the most common trans-
range from a fraction of centimeter to a few centime- verse field distribution of any output laser beam. For this
ters. The optical cavity is open to reduce drastically the reason the study of laser modes is closely related to the
number of modes that can oscillate with low loss. In propagation properties of Gaussian (or Gauss–Hermite)
fact, if the cavity were closed, the number N of res- beams.
onant modes that might oscillate, i. e., the number of
modes whose resonance frequency falls within the gain- Gaussian Beams
line of the active medium, is approximately given by The electric field of a monochromatic (and uniformly
N ≈ (8πν2 /c3 )V ∆ν0 , where (8πν2 /c3 ) is the density of polarized) light wave propagating at a small angle (i. e.,
modes, ∆ν0 the line width of the gain medium, and V paraxially) along the z-direction of an xyz cartesian
is the cavity volume. Note that V is usually several or- system of coordinates can be described as follows:
ders of magnitude larger than λ3 at optical wavelengths.
To estimate N, let us consider an active medium with E(x, y, z, t) = E 0 u(x, y, z) ei(ωt−kz) + c.c. , (11.26)
a narrow line width, such as the λ = 633 nm transition
of the HeNe laser (∆ν0∗ = 1.7 GHz). Assume a res- where ω = 2πν, ν is the optical frequency, k = 2π/λ is
onator length L = 50 cm closed by a lateral cylinder the wavenumber, λ is the optical wavelength, u(x, y, z)
with diameter 2a = 3 mm. The cavity volume is then is the complex field envelope obeying the so-called
V = πa2 L, and the number of cavity modes that fall paraxial wave equation, which in case of free-space
596 Part C Coherent and Incoherent Light Sources

 z
2
propagation reads R
R(z) = z 1 + , (11.30)
z
∂2u ∂2u ∂u  
+ 2 − 2ik =0. (11.27) z
∂x 2 ∂y ∂z ϕ(z) = tan−1 , (11.31)
zR
Among the solutions of (11.27) that retain their
where z R = πw20 /λ is a parameter referred to as the
functional form during propagation, the fundamental
Rayleigh range. Note that u(x, y, z) is given by the prod-
Gaussian beam solution turns out to be particularly
Part C 11.1

uct of three terms: an amplitude factor with a transverse


suited to describe laser beams both inside and outside
Gaussian distribution, (w0 /w) exp[−(x 2 + y2 )/w2 ] (see
the resonator [11.12]. A Gaussian beam is a solution of
Fig. 11.7a); a transverse phase factor, exp[−ik(x 2 +
the paraxial equation (11.27) of the form:
y2 )/(2R)]; and a longitudinal phase factor exp(iϕ). The
 2 
w0 x + y2 amplitude factor in (11.28) shows that, while propagat-
u(x, y, z) = exp − 2 ing, the beam intensity distribution retains its shape, but
w(z) w (z)
  its transverse size w, which is called the beam spot size,
x 2 + y2 changes along the propagation direction z according to
× exp −ik
2R(z) (11.29). Note that w(z) is a symmetric function of z with
× exp[iϕ(z)]. (11.28) a minimum spot size w = w0 at the plane z = 0, which
is hence referred to as√the beam waist (Fig. 11.7b). For
In the preceeding equation, w(z), R(z) and ϕ(z) are given z = z R , one has w = 2w0 so that the Rayleigh range
by z R represents the distance from the beam waist√ at which
 the beam spot size increases by a factor 2. At large
 2
z distances (i. e., for z z R ), w increases linearly with z,
w(z) = w0 1 + , (11.29)
zR according to w ≈ (w0 /z R )z. Hence we can define a beam
divergence due to diffraction as θd = limz→∞ w(z)/z,
obtaining
a) E (r) b) w/w0 λ
E0 θd = . (11.32)
4
πw0
The transverse phase factor in (11.28) has the same form
E0 /e 2 as that for a spherical wave in the paraxial approxima-
tion, R playing the role of the radius of curvature of the
èd
spherical wavefront. Thus, we can say that a Gaussian
w r 0 1 2 3 z/zR beam has an approximately spherical wavefront with
c) R/zR a radius of curvature varying along propagation accord-
ing to (11.30). Note that R(z) is an odd function of z
(Fig. 11.7c), showing a minimum Rmin = 2z R at z = z R ;
4 for z z R , R increases linearly with z, whereas one has
R → ∞ as z = 0. Thus the wavefront is flat at z = 0 and,
2 at large distances, its radius increases linearly with z just
as for a spherical wave. The longitudinal phase factor ϕ
–3 –2 –1
provides, in addition to the usual phase shift −kz of
1 2 3 z/zR
plane waves, a longitudinal phase shift (sometimes re-
2 ferred to as the Gouy phase shift), slowly varying with z
from −(π/2) to (π/2) on going from z  z R to z z R .
4 An important parameter of a Gaussian beam at
a given propagation plane z is the so-called complex-q
parameter, defined by the relation:
1 1 λ
Fig. 11.7a–c The fundamental Gaussian beam in free-space prop- = −i . (11.33)
agation: (a) the Gaussian transverse amplitude profile, being q R πw2
r = (x 2 + y2 )1/2 ; (b) the beam spot size w(z); (c) the wavefront It can be shown that, for a Gaussian beam propagating in
radius of curvature R(z) free space, the q parameter changes along propagation
Lasers and Coherent Light Sources 11.1 Principles of Lasers 597

according to

q(z) = z + iz R . (11.34)

TEM00 TEM10 TEM20


Equations (11.29) and (11.30) can indeed be obtained
upon inserting the parameter q from (11.33) into (11.34)
and then separating the real and imaginary part of the

Part C 11.1
resulting equation.
The fundamental Gaussian beam described above
belongs to a more general set of eigensolutions of (11.27)
which can be written as the product of an Hermite poly- TEM30 TEM50 TEM11
nomial with a Gaussian function. These are known as
Hermite–Gaussian beams, and assume the following
form [11.3, 5]
√  √ 
w0 2x 2y
u l,m (x, y, z) = Hl Hm
w(z) w(z) w(z) TEM21 TEM22 TEM23
 2 
x + y2 Fig. 11.8 Grey scale intensity patterns of a few low-order
× exp − 2
w (z) Hermite–Gaussian modes

x 2 + y2
× exp −ik z = z 2 , into the distribution
2R(z)  1+l+m
1
× exp[i(1 + l + m)ϕ(z)] , (11.35) u(x, y, z 2 ) =
A + (B/q1 )
√  √ 
where w(z), R(z) and ϕ(z) are given by (11.29, 30, 31), 2x 2y
respectively, and Hl , Hm are Hermite polynomials of or- × Hl Hm
w2 w2
der l and m. The lowest-order Hermite–Gaussian beam
is obtained by setting l = m = 0 in (11.35). These solu- × exp[−ik(x 2 + y2 )/(2q2 )] , (11.36)
tions are often referred to as TEMlm beams, where TEM where the values q1 and q2 of the complex-q parameter at
stands for transverse electric magnetic: within the parax- the input (z = z 1 ) and output (z = z 2 ) planes are related
ial approximation, both electric and magnetic fields of by the so-called ABC D law
the EM wave are, in fact, approximately transverse to the
Aq1 + B
z-direction. Note that, for a TEMlm beam, the number of q2 = . (11.37)
zeros of the field along the x- and y-directions is given Cq1 + D
by the subscripts l and m, respectively, and therefore As a particular case, note that for free-space propagation
the intensity distribution of the TEMlm beam consists of from z 1 = 0 to z 2 = z one has A = 1, B = z, C = 0, and
l + 1 lobes in the horizontal direction and m + 1 lobes in D = 1, so that the ABC D law (11.37) yields (11.34).
the vertical direction (Fig. 11.8).
As a final remark, it should be noted that Gauss– Optical Resonators: Introductory Concepts
Hermite beams maintain their functional shape as The simplest optical resonator is the plane-parallel or
they propagate along an arbitrary paraxial optical Fabry–Pérot resonator, consisting of two plane metallic
system, described by a paraxial ray matrix ABC D. or dielectric mirrors set parallel to one another [11.13].
Beam propagation, in this case, is simply ruled by At first approximation, the modes of this resonator can be
an algebraic relation for the complex q parameter of considered as the superposition of two plane EM waves
the Gaussian beam, which is known as the ABC D propagating in opposite directions along the cavity axis
law. In fact, if z = z 1 and z = z 2 are the input and (Fig. 11.9a). In this approximation, resonance frequen-
output planes of the ABC D paraxial optical sys- cies can be readily obtained by imposing the condition
tem,√a Gauss–Hermite
√ field distribution u(x, y, z 1 ) = that the cavity length L must be an integer multiple of
Hl ( 2x/w1 )Hm ( 2y/w1 ) exp[−ik(x 2 + y2 )/(2q1 )] at half-wavelengths, i. e., L = n(λ/2), where n is a posi-
the input plane z = z 1 is transformed, at the output plane tive integer. This is a necessary condition for the electric
598 Part C Coherent and Incoherent Light Sources

field of the EM standing wave to be zero on the two, e.g. some arbitrary distance L (Fig. 11.9b). These resonators
metallic, mirrors. It follows that the resonant frequencies can be divided into two categories: stable resonators
are given by and unstable resonators. A resonator is said to be un-
c
stable when, in bouncing back and forth between the
νn = n . (11.38) two mirrors, an arbitrary paraxial ray diverges indefi-
2L
nitely away from the resonator axis, either radially or
Note that (11.38) can also be obtained by imposing the
angularly. Conversely, a resonator whose paraxial rays
condition that the phase shift of a plane wave due to
Part C 11.1

remain bounded is said to be stable. An example of an


one round-trip through the cavity must equal an inte-
unstable resonator is shown in Fig. 11.9c. Among stable
gral number times 2π, i. e., 2kL = 2nπ. This condition
spherical resonators, symmetric resonators (i. e., hav-
is readily obtained by a self-consistency argument: if the
ing R1 = R2 ) are of particular importance; the confocal
frequency of the plane wave is equal to that of a cav-
resonator, in which the two spherical mirrors have the fo-
ity mode, the phase shift after one round-trip must be
cus in common (R1 = R2 = L), is a noteworthy example
zero (apart from an integer multiple of 2π). Only in this
of a spherical symmetric resonator. Another important
case, in fact, do the amplitudes at any arbitrary point,
scheme for laser cavities is that employing a ring res-
due to successive reflections, add up in phase to give
onator, where the path of the optical rays is arranged
an appreciable total field. According to (11.38) the fre-
to form a closed loop (Fig. 11.9d). Also in this case the
quency difference between two consecutive modes, i. e.,
resonant frequencies can be obtained by imposing the
differing by 1 in the longitudinal mode index n, is given
condition that the total phase shift along the ring path
by
must equal an integer number of 2π. The expression
c for the resonance frequencies of longitudinal (or axial)
∆ν = . (11.39)
2L modes is thus given by
This difference is referred to as the frequency difference  
c
between two consecutive longitudinal (or axial) modes. νn = n (11.40)
Note that, since the number n indicates the number of Lp
half-wavelengths of the mode along the resonator axis, where L p is the length of the closed loop path. In
the two consecutive modes have a different longitudinal general, a standing-wave pattern may be formed in
pattern. ring resonators, because the beam can propagate either
A more general class of laser resonators is the one clockwise or counterclockwise along the loop. Anyway,
made of spherical resonators, which are formed by two unidirectional ring resonators can be realized by means
spherical mirrors of radius of curvatures R1 and R2 , of optical diodes inserted along the beam path.
either concave (R > 0) or convex (R < 0), placed at
Stability Condition
In general, a laser cavity can be viewed as made of two
a) b) spherical mirrors comprising a set of intermediate op-
R2
tical elements like lenses, mirrors, prisms, and so on
R1
(Fig. 11.10a). If we define an arbitrary plane β orthog-
C2 C1 onal to the cavity optical axis, it is intuitive (and can
be rigorously demonstrated) that the round-trip propa-
L

c) d) a) b)
â â â

Cavity r0 r1
A B
optical
elements C D

L 2L

Fig. 11.9 (a) Plane-parallel resonator; (b) Spherical two- Fig. 11.10 (a) A general laser cavity, and (b) its equivalent
mirror resonator; (c) An unstable resonator; (d) A unidirec- representation given by resonator unfolding with respect to
tional ring resonator an arbitrary β plane
Lasers and Coherent Light Sources 11.1 Principles of Lasers 599

gation along the cavity is equivalent to the propagation


g2
in a suitable optical system S having β as input and
output planes, a transformation known as the unfolding g 1g 2 = 1
of the resonator. Paraxial propagation in such a sys-
tem can be described by means of the ABC D cavity b
round-trip matrix (Fig. 11.10b). Accordingly, if we let C
r0 and r0 be, respectively, the transverse coordinate and

Part C 11.1
angle that a ray make with the optical axis when in-
B g1
tercepting plane β at time t = 0, and rn and rn be the
coordinate of the same ray after n cavity round-trip, we A
have
n

rn A B r0 n r0 g 1g 2 = 1
= =M . (11.41)
rn C D r0 r0
Therefore, the optical resonator is stable if and only
if, for any initial set of coordinates (r0 , r0 ), the cor- Fig. 11.11 Stability diagram for a general two-mirror spher-
responding coordinates (rn , rn ) do not diverge as n ical resonator. Stable resonators correspond to (g1 , g2 )
increases. This condition is met provided that the eigen- points lying in the gray region of the plane
values λ1,2 of M are, in modulus, not larger than
one. Since λ1,2 = exp(±iθ), where cos(θ) = (A + D)/2, The stability condition given by (11.44) can be con-
the stability condition requires that θ be real, i. e., veniently displayed in the (g1 , g2 )-plane as reported
that in Fig. 11.11. Stable resonators correspond to those

A+ D points in the gray region of the plane, excluding those

2 1. (11.42) which lie on the boundaries, (i. e., satisfying the con-
ditions g1 g2 = 0 or g1 g2 = 1), which are referred to
For the particular case of two-mirror resonators, we as marginally stable resonators. Note that symmetric
can go one step further by explicitly calculating the cor- resonators (i. e., having mirrors of the same radius of
responding ABC D matrix. We recall that a given overall curvature R1 = R2 = R) lie on the bisector line b. As
matrix can be obtained by the product of matrices of in- particular examples of these symmetric resonators, one
dividual optical elements traversed by the beam, with can see that those corresponding to point A, B and C of
the matrices written in the reverse order compared to the figure are the concentric (L = 2R), confocal (L = R)
ray propagation through the corresponding elements. In and plane (R = ∞) resonators, respectively. Since points
our case, the ABC D matrix is then given by the or- A, B and C lie on the boundary of the stability region,
dered product of the following matrices: reflection from the corresponding resonators are only marginally stable.
mirror 1, free-space propagation from mirror 1 to 2,
reflection from mirror 2, free-space propagation from Laser Modes
mirror 2 to 1: The modes of an optical resonator are defined as the sta-

tionary (i. e., monochromatic) or weakly damped field
A B 1 0 1 L 1 0 1 L
= . distributions that can be sustained inside the cavity and
C D −2/R1 1 0 1 −2/R2 1 0 1
that satisfy the boundary conditions imposed by the cav-
ity mirrors. We note that, in open resonators, diffraction
After performing matrix multiplication we obtain losses due to the finite aperture of the mirrors make the
  
A+ D L L modes always leaky. The electric field for a mode in
= 1− 1− −1 . (11.43)
a leaky resonator can then be generally represented as
2 R1 R2
It is customary to define dimensionless quantities, re- E(x, y, z, t) = a(x, y, z) cos(ωt)

ferred to as the g1 and g2 parameters, defined as −t
g1 = 1 − L/R1 and g2 = 1 − L/R2 . In terms of these × exp (t > 0) , (11.45)
2τc
parameters, the stability condition transforms into the
where a(x, y, z) is the mode field distribution, ω is the
very simple relation:
resonance frequency, and τc describes field decay due
0 < g1 g2 < 1 . (11.44) to cavity losses and is referred to as the cavity pho-
600 Part C Coherent and Incoherent Light Sources

ton lifetime. In order to determine the resonator modes, when a point-like source at the (x1 , y1 ) point is
the corresponding resonance frequencies and diffraction placed at the z = 0 input plane. Indeed, if Ẽ(x1 , y1 , 0)
losses let us consider the rather general class of res- were a bidimensional Dirac δ-function centered at
onators with an optical axis z, as shown in Fig. 11.10a. x1 = x1 and y1 = y1 , i. e., if Ẽ(x1 , y1 , 0) = δ(x1 −
Propagation of an EM wave back and forth between x1 , y1 − y1 ), then from (11.46) one would readily get
the two end mirrors of the cavity is equivalent to the Ẽ(x, y, 2L) = K (x, y; x1 , y1 ) exp(−2ikL). For a gen-
unidirectional propagation of an EM wave in a peri- eral optical system, the calculation of the kernel K
Part C 11.1

odic sequence of optical elements (e.g., a lens guide) is usually rather complicated. However, within the as-
which is obtained by unfolding the resonator, as shown sumption of infinite aperture of all optical elements, the
in Fig. 11.10b. Note that, in the unfolding scheme, the kernel K is simply expressed in terms of the round-
end spherical mirrors should be replaced by thin spheri- trip resonator-matrix elements ABC D by the relation
cal lenses with focal length equal to the mirror radius of (Huygens–Fresnel–Kirchhoff kernel)
curvature.
Let us first consider the propagation of a monochro- K (x, y; x1 , y1 )

matic EM field in a periodic lens guide. By i ik
= exp −
writing the electric field along the lens guide as λB 2B
E(x, y, z, t) = Ẽ(x, y, z) eiωt + c.c., due to the linear-  
ity of the Huygens–Fresnel integral the complex field × A(x12 + y12 ) + D(x 2 + y2 ) − (2xx1 + 2yy1 )
amplitude Ẽ after one period of the lens guide can gen- (11.47)
erally be written by an integral transformation, namely
(Fig. 11.12) and the integral in (11.46) can be extended from −∞
to ∞.
Ẽ(x, y, 2L) Let us now define a mode of a periodic lens
= exp(−i2kL) guide as a field distribution which reproduces itself

after one guide period except for an overall ampli-
× K (x, y; x1 , y1 ) Ẽ(x1 , y1 , 0) dx1 dy1 , (11.46) tude reduction, due to lens-guide losses, and a phase
1 shift ∆ϕ accounting for field propagation. Hence
where K (x, y; x1 , y1 ) is a function of the transverse co- Ẽ(x, y, 2L) = |σ̃| exp(i∆ϕ) Ẽ(x, y, 0), where |σ̃| < 1.
ordinates of both input and output planes, known as It is now convenient to write the phase shift as
the propagation kernel. Note the phase term (−2kL), ∆ϕ = −2kL + ϕ, where −2kL is the shift of a plane
which represents the phase shift if the wave were wave and ϕ is an additional phase term due to the fact
a plane wave. The kernel K accounts for all the that the lens-guide mode is not a plane wave. Hence, for
elements encountered during propagation from in- a lens-guide mode we require the condition
put plane 1 (z = 0) to output plane 2 (z = 2L) and Ẽ(x, y, 2L) = σ̃ exp(−2ikL) Ẽ(x, y, 0) , (11.48)
represents, from a physical viewpoint, the field dis-
tribution observed at the (x, y)-plane (i. e., at z = 2L) where σ̃ = |σ̃| exp(iϕ). Substitution of (11.48) into
(11.46) yields

~
K (x, y; x1 , y1 ) Ẽ(x1 , y1 , 0) dx1 dy1
1 E (x1, y1, 0) 2
1
y1 y = σ̃ Ẽ(x, y, 0) . (11.49)

x1 x Note that the mode distribution Ẽ(x, y, 0) is an eigen-


0 2L z function of a Fredholm homogeneous integral equation
Optical of the second kind corresponding to the eigenvalue σ̃. As
system a rather general property, it turns out that the Fredholm
S ® K (x1, y1; x, y) ~ integral equation admits a doubly infinite discrete set of
E (x, y, 2L)
confined eigensolutions, which can be distinguished by
a pair of integer positive numbers l and m. Accordingly,
Fig. 11.12 Field calculation at plane 2 (z = 2L) when the field the corresponding eigenvalues will generally be indi-
Ẽ(x1 , y1 , 0) at plane 1 (z = 0) is known cated as σ̃lm = |σ̃lm | exp(iϕlm ), with |σ̃lm | < 1 owing to
Lasers and Coherent Light Sources 11.1 Principles of Lasers 601

the overall losses (namely, diffraction losses, scattering loss mechanisms are always present in a laser resonator.
losses from optical elements, and so on) encountered in For instance, the mirror reflectivity of the output coupler
one period of propagation along the lens guide. is always smaller than 100%, which means that a frac-
Now, let us return to the problem of cavity mode tional part of the photons φ stored in the cavity escapes
calculation. In this case, the mode Ẽ of the lens guide from the resonator at each round-trip. Scattering or ab-
corresponds to a mode of the resonator of Fig. 11.10a sorption losses of intracavity optical elements are also
provided that, after one cavity round-trip, the overall another common cause of photon leakage. To calculate

Part C 11.1
phase shift ∆ϕ accumulated in one cavity round-trip the rate of energy decay in a given cavity mode, let I0 be
is zero apart from an integer number of 2π, i. e., the initial intensity corresponding to the field amplitude
∆ϕ = −2kL + ϕlm = −2πn. From this condition and at a fixed point within the cavity, and let R1 and R2 be
using the relation k = 2πν/c between the wavenumber the (power) reflectivities of the two mirrors and L i the
k and frequency ν of the mode, one readily obtains the fractional internal loss per pass, which accounts for scat-
cavity resonance frequencies as tering, absorption and diffraction losses. The intensity
c ϕlm
at the same point, after a round-trip time τR = 2L e /c,
νnlm = n+ . (11.50) is I(τR ) = R1 R2 (1 − L i )2 I0 = I0 exp(−2γ ), where L e is
2L 2π
the cavity optical length and γ is the logarithmic loss
Note that we have indicated explicitly that these frequen- per pass, defined by the relation
cies depend on the three integer numbers l, m, and n. The
integers l and m define the transverse field profiles of the γ1 + γ2
γ= + γi (11.52)
mode (Fig. 11.8), i. e., they represent the number of zeros 2
of the field along the x- and y-coordinates, respectively. with γ1 = −ln(R1 ), γ2 = −ln(R2 ), and γi = −ln(1 −
The integer n defines the longitudinal field configura- L i ). In view of the exponential decay law introduced
tion, i. e., the number of zeros of the EM standing wave in (11.45), after a round-trip time we must have
(nodes) as previously discussed for the plane-parallel I(τR ) = I0 exp(−τR /τc ), and thus we conclude that the
resonator (11.38). photon lifetime is given by
For stable resonators with infinite apertures the
eigenmodes of the Fredholm equation are given by τR Le
τc = = . (11.53)
the Gauss–Hermite functions, and their resonance fre- 2γ cγ
quencies can be calculated from (11.50) using the Having calculated the photon lifetime, the time
propagation law (11.36). For instance, for the impor- behavior of the electric field at any point inside the res-
tant case of two-mirror spherical resonators, it turns out onator can be written as E(t) = E 0 exp(−t/2τc + iωt) +

that ϕlm = 2(1 + l + m) cos−1 (± g1 g2 ), where the plus c.c., where ω is the angular frequency of the mode. The
or minus sign depends on whether g2 (and hence g1 ) is same time behavior then applies for the field of the wave
positive or negative. The resonance frequencies of the leaving the resonator through the output mirror. Taking
two-mirror spherical resonator are thus given by: the Fourier transform of this field (for t > 0) we find that

c 1+l +m −1 √ the power spectrum of the emitted light has a Lorentzian
νnlm = n+ cos (± g1 g2 ) . line shape with line width (FWHM) given by
2L π
(11.51) 1
∆νc = . (11.54)
For, e.g., a confocal resonator, one has g1 = g2 = 0, 2πτc
and hence νnlm = [c/(4L)](2n + 1 + l + m). Note that We can now introduce an important quality factor which
modes with the same value of (2n +l + m) have the same is strictly related to the photon lifetime. This is the cavity
resonance frequency, and they are said to be frequency Q-factor which is defined, for any resonant system, as
degenerate. Note also that, for a confocal resonator, the 2π times the ratio between the energy stored in the res-
mode spacing is c/(4L). onator and the energy lost in one oscillation cycle. Thus
a high cavity Q-factor implies low losses in the resonant
Photon Lifetime and Cavity Q system. Since in our case the energy stored is φhν and
The modes of an optical resonator are always leaky and the energy lost per cycle is (− dφ/ dt)h we obtain
therefore show a finite photon cavity lifetime τc . In fact,
besides diffraction losses due to finite aperture effects 2πνφ ν
Q=− = , (11.55)
of mirrors or intracavity optical elements, some other dφ/ dt ∆νc
602 Part C Coherent and Incoherent Light Sources

where the exponential decay law φ(t) = φ0 exp(−t/τc ) of photons φ of the oscillating mode stored in the cavity:
for the stored cavity photons φ has been used and where dN N
the expression for ∆νc given by (11.54) has also been = Rp − BφN − (11.56)
utilized. dt τ
dφ φ
As an example, consider a two-mirror spherical res- = − + Va BφN , (11.57)
onator with R1 = R2 = R = 0.98 and assume L i  0. dt τc
From (11.53) we obtain τc = τT /[−ln(R)] = 49.5 τT , where Rp is the pump rate per unit volume, τ is the
Part C 11.1

where τT = L/c is the transit time of the photon for lifetime of the upper laser level 2, and τc is the photon
a single pass in the cavity. Note that the photon life- lifetime for the oscillating mode. In (11.56), the terms
time is much longer than the transit time, a typical Rp , N/τ and BφN = W21 N account for the pumping
result of low-loss cavities. If we now assume L = 90 cm, process, radiative and nonradiative decay, and stimulated
we get τT = 3 ns and τc  150 ns. From (11.54) we emission, respectively. The constant B, which represents
can then calculate ∆νc  1.1 MHz. Finally, assuming the stimulated transition rate per photon, per mode is re-
a laser wavelength λ  630 nm corresponding to an op- lated to the transition cross section σ by the simple
tical frequency ν = 5 × 1014 Hz, from (11.55) we have equation B = σc/V , where V is the mode volume in
Q = 4.7 × 108 . Thus laser resonators have a remark- the laser cavity [11.3]. The first term on the right-hand
ably high Q-value, which means that a very small side in (11.57), φ/τc , represents the number of cavity
fraction of the energy is lost during one oscillation photons that are lost per unit time due to internal loss,
cycle. diffraction loss and output coupling through the mirrors.
Finally, the second term in (11.57) represents the number
11.1.4 Laser Rate Equations of photons (per unit time) that are created in the oscil-
and Continuous-Wave Operation lating mode owing to stimulated emission: since BφN
represents the number of atoms per unit volume and per
A simple and powerful approach for understanding the unit time that decay creating a photon in the oscillat-
basic dynamical behavior of a laser is based on a rate- ing cavity mode, the total number of photons created
equation model, in which simple balance equations for per unit time can be expressed as the product of BφN
the total number of atoms undergoing a transition and with the volume Va occupied by the cavity mode inside
the total number of photons created or annihilated are the gain medium. Spontaneous emission in not included
written [11.3]. For a more-refined treatment of laser dy- in the balance equation (11.57) since only a negligi-
namics based on either a semiclassical or a full-quantum ble fraction of spontaneously emitted photons belongs
electrodynamic approach, which may account for certain to the oscillating mode. However, spontaneous emission
phenomena such as dynamical laser instabilities, laser photons are important to allow laser action starting.
coherence and photon statistics, we refer the reader to The laser output power Pout is related to the photon
more-specialized literature [11.6, 8]. number φ by the simple relation
γ2 φ γ2 c
Laser Rate Equations Pout = (hν) = hνφ . (11.58)
Let us consider a four-level laser scheme (Fig. 11.4b) 2γ τc 2L e
and make the following assumptions: In fact, (hν)(φ/τc ) is the total EM energy lost in the
cavity per unit time, and solely a fraction γ2 /(2γ ) of
1. the laser transition is homogeneously broadened, this power is available due to transmission through
2. the lifetime τ1 of the lower laser level 1 is short the output mirror. For a typical CW laser operated in
enough that we may neglect the population in level 1, the continuous-wave regime, the number of photons φ
3. a single longitudinal and transverse mode is oscil- stored in the cavity may vary from about 1010 photons
lating in the cavity, for low-power lasers (such as a HeNe laser delivering
4. we neglect the precise transverse and longitudinal Pout = 10 mW power at λ = 632.8 nm) to 1017 photons
spatial variation of the cavity mode, for high-power lasers (such as a CO2 laser delivering an
5. we assume uniform pumping of the active medium. output power Pout = 10 kW at λ = 10.6 µm).

Under these assumptions, we can write the fol- Threshold Condition


lowing rate equations for the population inversion The population inversion needed to reach the threshold
N = N2 − N1  N2 in the active medium and the number for laser oscillation is simply obtained from (11.57) by
Lasers and Coherent Light Sources 11.1 Principles of Lasers 603

imposing dφ/ dt = 0. An initially small number of pho-


N, ö
tons turns out to be exponentially damped for N < Nc
or exponentially amplified for N > Nc , where:
Nc N
1 γ
Nc ≡ = (11.59)
τc BVa σl ö
is referred to as the critical inversion (or threshold

Part C 11.1
inversion). In this equation, l is the length of the ac-
tive medium and the threshold condition σ Ncl = γ
is reached when the gain in the inverted medium, 0
g = σ Nl, equals the logarithmic loss γ of the cavity. Rcp Rp
Laser below Laser above
The pump rate corresponding to the threshold condi- threshold threshold
tion is Rcp = Nc /τ = γ /(σlτ); the corresponding pump
power at threshold Pth is then obtained using (11.9). The Fig. 11.13 Behavior of population inversion N and photon
perturbation that starts the laser action when the pump number φ in the oscillating mode versus the pump rate Rp
rate Rp reaches the critical value Rcp is provided by for a four-level laser. Rcp is the critical pump rate above
spontaneous emission. which laser action takes place

Output Power and Slope Efficiency bation of the system (e.g., of cavity losses) is damped.
For a pump rate Rp > Rcp , the rate equations (11.56, 57) When the ratio τ/τc between the upper laser level life-
admit the solution N0 = Nc and φ0 = [1/(Bτ)](x − time and cavity photon lifetime is larger than 1 (or much
1), corresponding to laser being above threshold larger, such as in laser transitions which are electric-
(Fig. 11.13). Here x = Rp /Rcp = Pp /Pth > 1 is the dipole forbidden), relaxation to the steady state occurs
above-threshold pump behavior parameter, where Pp is through damped oscillations in both photon number and
the pump power and Pth is its threshold value. The cor- population inversion. This results in damped oscillations
responding output laser power can be then calculated of the output power referred to as relaxation oscilla-
from (11.58) and can be cast in the form tions. In solid-state lasers, the frequency of relaxation
Pout = ηs (Pp − Pth ) , (11.60) oscillations typically fall in the 10 kHz–10 MHz region,
whereas, in semiconductor lasers, it falls in the GHz re-
where gion. Relaxation oscillations in slow-gain media (such
as in solid-state lasers) triggered by technical noise or
ηs = ηp ηc ηq ηt . (11.61)
by pump power fluctuations are one of the major cause
Equation (11.60) shows that, within the approximation of amplitude noise in the output laser power. Whenever
made, a linear relation is obtained between the output a high degree of intensity stability is required, laser am-
power and the pump power. One can then define the slope plitude stabilization may be provided by a suitable active
efficiency of the laser as ηs = dPout / dPp . According to feedback loop.
(11.61), ηs is given by the product of four contributions:
Laser Tuning
1. the pump efficiency ηp
The gain line width of some lasers (e.g., dye lasers or
2. the output coupling efficiency ηc = γ2 /(2γ )
vibronic solid-state lasers) is very wide and, for sev-
3. the laser quantum efficiency ηq = (hν)/(hνmp )
eral applications, one needs to tune the laser output
4. the transverse efficiency ηt = Ab /A
wavelength away from the line center and across the
where Ab = Va /l is the transverse mode area in the active entire available line width. In other cases, different las-
medium and A the transverse pumping area. The slope ing transitions may compete or may potentially be used,
efficiency of a laser may typically vary from less than and one needs to select one of them. In both circum-
1% in low-efficiency lasers (such as in the HeNe laser) stances, one can employ a wavelength-selective element
to 20–50% or even higher in high-efficiency lasers. inside the laser cavity, which is often referred to as
laser tuner. For lasers in the middle infrared (such as
Relaxation Oscillations CO2 lasers), one generally uses a diffraction grating
One can show that the solution, given above, for lasers in the so-called Littrow configuration (Fig. 11.14a) as
above threshold is stable, i. e., that any initial pertur- one of the cavity mirror. Wavelength tuning is simply
604 Part C Coherent and Incoherent Light Sources

birefringent plate does not change the polarization state


a) of the beam and thus allows for laser oscillation with
Gain medium ë2 low loss. Upon rotation of the plate around the axis or-
thogonal to its faces (Fig. 11.15) the direction of the
birefringence axes of the plates is changed and this cor-
ë1 respondingly changes the wavelength at which low loss
occurs.
Part C 11.1

Mirror Grating Single Mode Selection


b) and Limit to Laser Monochromaticity
Most often, lasers tend spontaneously to oscillate on sev-
Gain medium eral transverse and longitudinal modes, especially when
ë2
the gainline is relatively broad. The reasons for mul-
timode oscillations are rather involved and their study
goes beyond the scope of the present contribution. For
ë1 many applications, single-mode operation may be re-
Prism
Mirror Mirror
quired, and therefore one needs to force the laser to
oscillate on a single transverse (usually the fundamen-
Fig. 11.14 (a) Laser tuner based on a diffraction grating in tal TEM00 Gaussian mode) and longitudinal mode. For
the Littrow configuration. (b) Laser tuner based on the use stable resonators, single transverse mode oscillation is
of a dispersive prism easily achieved by placing an aperture inside the cav-
ity of appropriate size in order to increase diffraction
achieved by grating rotation. In the visible or near- loss of higher-order modes with respect to the TEM00
infrared spectral regions (such as for the Ar3+ laser), mode. In some cases, such as in longitudinally pumped
a dispersive prism is more commonly used and wave- solid-state lasers, limitation on the pump spot size lends
length tuning is simply achieved by prism, or mirror, itself to TEM00 mode selection.
rotation (Fig. 11.14b). To reduce insertion losses, the Even when a laser is oscillating on a single trans-
two prisms facets are approximately inclined at Brew- verse mode, it can still oscillate on several longitudinal
ster angle. A third wavelength-selective element, which modes. This usually occurs since the longitudinal-mode
is becoming increasingly popular in the visible or near- separation ∆ν = c/(2L) is smaller (or much smaller)
infrared, uses a birefringent filter inside the cavity. than the gain line width ∆ν0 . For some gas lasers,
This device exploits a birefringent plate, inclined at where the gain line width is relatively small (up to a few
the Brewster angle, which generally changes the po- GHz), single-longitudinal-mode selection is simply ob-
larization state of the intracavity laser beam. In the tained by making the cavity length short enough that the
presence of an intracavity polarizer, or just exploiting longitudinal-mode separation ∆ν becomes larger than
the polarizing properties of the Brewster-angle filter, the ∆ν0 /2. For, e.g., a HeNe laser (∆ν0∗  1.7 GHz), this
birefringence filter thus generally produces additional condition implies L ≤ 17.5 cm. For solid-state lasers
cavity losses. However, at certain wavelengths, λ, the with a bandwidth up to a few hundred GHz, this condi-
tion requires cavity lengths in the sub-millimeter region
(microchip lasers). For lasers with much larger band-
Rotation widths (e.g., dye lasers or tunable solid-state lasers),
for tuning
Birefringent the required length is too small to make the tech-
Brewster plate Resonator nique of practical relevance and to make the gain in
angle axis the medium large enough to reach threshold. In these
cases, different techniques are employed. For solid-
state or dye lasers, the simplest method is to use one
Polarizer
(or more) Fabry–Pérot etalons within the cavity, which
acts as a narrow frequency spectral-selective element
Mirror
(Fig. 11.16). The etalon thickness and finesse should be
Fig. 11.15 Schematic of a birefringent laser tuner made of designed to ensure single mode selection. This implies
an intracavity birefringent plate and polarizer that:
Lasers and Coherent Light Sources 11.1 Principles of Lasers 605

1. the half width ∆νFP /2 of the transmission peaks


Gain line
of the Fabry–Pérot must be smaller than the ÄíFSR
longitudinal-mode separation ∆ν = c/(2L); Fabry Perot
transmission
2. the etalon free spectral range ∆νFSR must be peaks
Äí0
larger than the half width of the gain line ∆ν0 /2
(Fig. 11.16). ÄíFP

For semiconductor lasers, single mode selection is

Part C 11.1
achieved by using a distributed feedback (DFB) struc- c í
ture, in which a longitudinal corrugation of the 2L
refractive index in the semiconductor induces fre-
Fig. 11.16 Schematic of single longitudinal mode selection by use
quency mode selection according to Bragg scattering
of an intracavity Fabry–Pérot etalon
theory.
A special case of single mode selection that deserves
∆L by just ≈ 10−8 times the atomic dimension leads to
mention is that of a laser with a homogeneously broad-
a contribution to ∆νL comparable to the quantum limit.
ened line (e.g., Nd:YAG and dye lasers). In this case,
Conversely, in semiconductor lasers the quantum limit
multimode oscillation is mainly due to the standing-
of ∆νL is considerably larger and typically falls in the
wave character of the laser mode arising from the
MHz range, owing to the much short photon lifetime (τc
interference of counter-propagating waves established
is of the order of few ps). Therefore, the laser line width
between the two cavity mirrors. The use of a ring
of a typical semiconductor laser arises from quantum
resonator instead of a linear cavity, in which unidirec-
noise.
tional operation is forced by, e.g., an intracavity optical
diode, may be enough in this case to achieve single
11.1.5 Pulsed Laser Behavior
longitudinal-mode operation.
We finally discuss the limit of monochromaticity
In lasers operating in the CW or quasi-CW regimes, the
(and hence of temporal coherence) of a laser. The line
maximum achievable optical output power is limited by
width ∆νL of a laser that oscillates on a single longi-
the maximum available pump power. For high-power
tudinal mode is ultimately established by spontaneous
CW lasers (such as CO2 lasers), power levels up to
emission noise. The quantum theory of a laser shows
≈ 100 kW can be reached; however larger power lev-
that the spectral shape of emitted light is Lorentzian with
els, which can be of interest for many applications, are
a FWHM given by the well-known Schawlow–Townes
prevented in the CW regime. Transient laser behavior al-
formula:
lows one to obtain higher peak powers by concentrating
N2 2πhνL (∆νC )2 the available energy in a single, short optical pulse or in
∆νL = , (11.62)
N2 − N1 P a periodic sequence of optical pulses [11.3,5]. Addition-
where P is the output power, ∆νC = 1/(2πτc ) is the line ally, transient laser behavior is a powerful tool for the
width of the cold cavity mode, N2 and N1 are the steady- generation of ultrashort optical pulses, with durations
state populations in the upper and lower laser levels, down to ≈ 10 fs in lasers with a broad gainline (notably
respectively, and νL is the emission frequency. Typi- the Ti3+ :Al2 O3 laser). From a dynamical viewpoint,
cally the line width predicted by the Schawlow–Townes pulsed laser behavior can be divided into two rather
formula is negligibly small compared to that produced distinct categories:
by other cavity disturbances (e.g., fluctuations of cavity
length or technical noise), except for the very important 1. Laser transients occurring on a time scale of the or-
class of semiconductor lasers. For, e.g., a typical HeNe der of the cavity photon lifetime τc , i. e., appreciably
laser oscillating on its red transition (λ = 632.8 nm), τc larger than the cavity round-trip time. This in-
is of the order of tens of µs, so that ∆νL is of the or- cludes the so-called Q-switching and gain-switching
der of  1 mHz, which turns out to be much smaller regimes, which enable the generation of optical
than the line broadening due to technical noise. For in- pulses as short as a few nanoseconds with optical
stance, a small cavity length change ∆L, due to technical peak powers typically in the megawatt range. These
noise, contributes to the frequency broadening ∆νL by are basically single-longitudinal-mode regimes and
an amount given by |∆νL | = (∆L/L)νL ; for L = 1 m can be described by means of a rate equation model
and νL = 4.7 × 1014 Hz (visible transition), a change of (11.56, 57).
606 Part C Coherent and Incoherent Light Sources

2. Laser transients occurring on a time scale appre- to pumping. When the shutter is opened, the Q factor
ciably shorter (and often much shorter) that the is suddenly switched to a high value and the laser ex-
cavity round-trip time. These are basically multi- hibits a gain g = σlN that greatly exceeds the loss γ .
longitudinal-mode regimes, i. e., they involve the Light emission then occurs via the generation of a short
simultaneous oscillation of many longitudinal laser and intense laser pulse. The duration of a Q-switching
modes, and include the so-called mode-locking pulse typically ranges from a few nanoseconds to a few
regime, which enables the generation of trains of tens of nanoseconds, whereas its peak power is in the
Part C 11.1

ultrashort laser pulses with durations down to a few megawatt range. To achieve sufficient population inver-
femtoseconds. sion when laser action is prevented, a long lifetime τ of
the upper laser level is required. Thus Q-switching can
Laser Q-switching: Dynamical Aspects be effectively used for electric-dipole-forbidden laser
Q-switching is a technique that enables the generation transitions, where τ generally falls in the millisecond
of a short optical pulse (of the order of the cavity photon range. This is the case of most solid-state lasers (e.g.,
lifetime τc ) by a sudden switching of the cavity Q factor, Nd, Yb, Er in different host materials; Cr-doped mater-
i. e., of the cavity loss γ . The change of Q is produced, in ials, such as alexandrite, Cr:LiSAF, and ruby) and some
principle, upon placing inside the laser cavity an opaque gas lasers (e.g., CO2 or iodine).
shutter which can be opened or closed. When the shut- To understand the basic dynamics of Q-switching,
ter is closed (i. e., the cavity Q is low), laser action is let us consider a four-level laser and assume that a step
prevented and the population inversion N can reach a rel- pump pulse is applied at time t = 0, i. e., Rp (t) = 0 for
atively large value (well above the critical value Nc ) due t < 0 and Rp = constant for 0 < t < tp , where tp is the
duration of the pump pulse; meanwhile the shutter is
closed (Fig. 11.17a) and laser action is prevented. From
a) (11.56) with φ = 0, one then obtains that the transient
Rp N population inversion increases accordingly to the rela-
Rp (t)
tion N(t) = N∞ [1 − exp(−t/τ)], where the asymptotic
N¥ value N∞ is given by N∞ = Rp τ (Fig. 11.17a). After
a pump time of about 2τ, the population inversion al-
ready reaches a value close to its asymptotic limit N∞ ,
N (t)
and therefore the pump pulse can be switched off and
the shutter opened. In fact, for tp larger than ≈ 2τ the
energy supplied to the medium is not useful for increas-
ô tp t
ing the population inversion any further but is lost as
b) radiative and nonradiative decay. Suppose now that the
N, ö Ni shutter is opened very rapidly at time tp (fast switching),
N (t) and take the origin of time at the instant when switching
occurs (Fig. 11.17b). From this time on, the evolution
of both population inversion and number of photons in
Nc
the cavity can be numerically computed by solving the
rate equations (11.56) and (11.57) with the initial con-
ö (t) ditions φ(0)  1 and N(0) = Rp τ[1 − exp(−tp /τ)] ≡ Ni ,
where the initial condition φ(0)  1 accounts for the fact
Nf that the laser action is started by spontaneous emission
Äôp
(the so-called extra photon). The qualitative transient
ôdelay t behavior of both N and φ is shown in Fig. 11.17b and
can be simply understood by observing that, just after
Fig. 11.17a,b Dynamics of fast switching in a four-level the switching time t = 0, the gain g = σ Nl in the gain
laser. (a) Temporal behavior of pump rate and population medium greatly exceeds the single-pass cavity loss γ ;
inversion when the cavity Q is low. (b) Temporal behavior therefore the number of photons, which increases nearly
of population inversion and cavity photons when the cav- exponentially with time starting from the extra photon
ity Q is suddenly switched to a high value, showing the due to spontaneous emission, typically takes from sev-
formation of the Q-switching pulse eral hundreds to a few thousand cavity round-trips to
Lasers and Coherent Light Sources 11.1 Principles of Lasers 607

reach a sufficient value to saturate the laser transition,


çE
thus producing a reduction of the available inversion
1
(Fig. 11.17b). This means that the time delay for the
peak of the laser pulse, τdelay typically ranges from sev- 0.8
eral tens to a few hundred of nanoseconds. Note that,
on such a time scale, the radiative and nonradiative 0.6
decays of the population N (which typically occur on
0.4

Part C 11.1
the millisecond time scale) are negligible, and therefore
population decay just occurs by stimulated emission. 0.2
The decrease of N as φ increases leads, in turn, to a de-
crease of the gain g = σ Nl. The peak of the pulse occurs 0
1 1.5 2 2.5 3 3.5 4
at the delay time, τdelay , such that the population inver- Ni/Nc
sion N decreases to its critical value, Nc . In this case, in
fact, laser gain g equals cavity loss γ and one has from Fig. 11.18 Behavior of the energy utilization factor ηE ver-
(11.57) dφ/ dt = 0. For t > τdelay , one has N < Nc and sus the normalized initial inversion Ni /Nc
dφ/ dt < 0. This means that the number of photons now
decreases towards zero. Meanwhile, due to stimulated of this energy, only the fraction [γ2 /(2γ )] goes into the
emission, the population inversion also keeps decreas- output beam.
ing until the photon pulse has decreased to zero. At Q-switched lasers may generally be operated in two
this time some population inversion, say Nf , is gener- distinct regimes. In so-called pulsed Q-switching, the
ally left in the medium after Q-switching (Fig. 11.17b). pump rate Rp (t) generally consists, as explained above,
Note that the quantity ηE = (Ni − Nf )/Ni represents the of a pulse with duration comparable to the upper-state
fraction of the energy initially stored in the material that lifetime τ. Of course, the pulsed operation can be pe-
goes into stimulated emitted photons, usually referred riodically repeated upon repeating the pulsed pump
to as the inversion, or energy, utilization factor. The du- (generally up to a rate of a few tens of Hz). In so-
ration ∆τp of  the Q-switched pulse, the output energy called CW repetitive Q-switching, the pump rate Rp is
E = (1/τc )[ φ(t) dt](hν)(γ2 /(2γ )), the energy utiliza- held constant and cavity losses are periodically switched
tion factor ηE , as well as the time τdelay needed for pulse from a high to a low value (generally with a rate from
formation can be derived in a closed form by an analysis a few to a few tens of kHz).
of the rate equations (11.56) and (11.57) in which pump- So far we have considered the dynamic behavior
ing and radiative and nonradiative decay are neglected. corresponding to fast switching, where the switching
One obtains: of the cavity loss is treated as instantaneous (in prac-
tice, much shorter than the time τdelay ). In the case of
(Ni /Nc )ηE slow switching, the dynamic behavior is somewhat more
∆τp = τc , (11.63)
(Ni /Nc ) − ln(Ni /Nc ) − 1 complicated and multiple pulses may result, as shown
 
γ2
E= (Ni ηE Va )(hν) , (11.64)
2γ g, ã, ö
τc
τdelay ≈ ln(φp /10) , (11.65)
(Ni /Nc ) − 1 ã (t)

where Ni /Nc is the ratio between the initially stored


population inversion and critical inversion; φp is the
peak photon number of the Q-switching pulse, given by
φp = Va (Ni − Nc ) − Nc Va ln(Ni /Nc ); and ηE is the en- g (t)
ergy utilization factor. The value of ηE can be calculated ö (t)
from the implicit equation (Ni /Nc )ηE = −ln(1 − ηE )
from which a plot of (Ni /Nc ) vs. ηE can readily be
obtained (Fig. 11.18). Note that (11.64) can readily be
t
obtained by a simple energy-balance argument: the
stored energy in the medium released as EM wave is Fig. 11.19 Gain and photon dynamics in a slow-switching
in fact equal to hν(Ni − Nf )Va = hν(ηE Ni )Va , and, out laser, showing the formation of multiple pulses
608 Part C Coherent and Incoherent Light Sources

in Fig. 11.19. In the figure, the behavior of the cavity crystal required to produce the phase shift ∆ϕ = π/2
loss γ and laser gain g = σ Nl is depicted. The multiple is referred to as the quarter-wave voltage and typically
intersections of the slowly decaying curve for the loss ranges from 1 to 5 kV. To avoid multiple pulses, this
γ (t) with the gain curve g(t) explain the formation of voltage must be switched off in a time typically smaller
multiple Q-switching pulses. than 20 ns.

Methods of Q-Switching Rotating prism. In this simple Q-switching technique,


Part C 11.1

Several methods have been developed to achieve switch- one of the cavity mirror is generally made of a roof-
ing of the cavity Q; the most common are [11.3, 4]: top prism and rotation is made through the axis parallel
to the other mirror and orthogonal to the prism edge
1. Electrooptic Q-switching;
(Fig. 11.21). The high-Q condition is achieved when
2. Rotating prism;
the prism edge passes through a position parallel to the
3. Acoustooptical Q-switching;
other cavity mirror. Although rotating prisms are simple
4. Saturable absorber Q-switching.
and inexpensive devices which can be used at any wave-
length, they suffer the limitation arising from the limited
Electrooptic Q-switching. In this case the shutter placed rotation speed (≈ 400 Hz). The Q-switching time is then
inside the laser cavity is made of a Pockels cell and rather long (typically ≈ 400 ns) which often results in
a polarizer in the configuration shown in Fig. 11.20 the production of multiple pulses (slow switching).
(electrooptic shutter). The Pockels cell consists of a suit-
able nonlinear electrooptic crystal (such as KD*P or Acoustooptic Q-switching. In this case the shutter
lithium niobate for the visible-to-near-infrared region or consists of an acoustooptic modulator, driven by a radio-
cadmium telluride for middle-infrared), in which an ap- frequency (RF) oscillator, which is placed inside the
plied dc voltage induces a change in the crystal refractive laser cavity. The modulator consists of a transparent
indices. The induced birefringence turns out to be pro- block of material (usually fused quartz in the visi-
portional to the applied voltage. The transmission axis ble to near-infrared or cadmium selenide in the mid-
of the polarizer is set at 45o with respect to the birefrin- to far-infrared) bonded on one side to a piezoelectric
gence axes of the crystal. When no dc field is applied transducer and to an acoustic absorber on the other
to the crystal, no polarization losses are introduced in (Fig. 11.22). When the transducer is on, traveling sound
the cavity by the electrooptic shutter, i. e., cavity losses waves are then produced in the material in the direc-
are low. However, when a dc field is applied such that tion orthogonal to the plane of the transducer. Due to the
the phase difference ∆ϕ between the ordinary and ex- photoelastic effect, the resulting strain in the material
traordinary waves in the birefringent-induced crystal is results in local changes of the material refractive index,
equal to π/2, the Pockels cell operates as a λ/4 bire- i. e., in the generation of an index grating which is travel-
fringent plate. Therefore, the linearly polarized light, ing along the material itself. Bragg scattering of the laser
coming from the polarizer, is rotated by 90◦ after a dou-
ble pass through the cell and it is then fully reflected out
of the cavity by the polarizer. The electrooptic shutter is Rotating
prism
now closed and cavity Q is zero. The dc voltage to the

E Voltage
Polarizer Gain medium
Electro-
Gain optic
medium Rotation
crystal axis Mirror

Mirror Mirror

Fig. 11.20 Schematic of a Q-switched laser using a Pockels Fig. 11.21 Schematic of a Q-switched laser using a rotating
cell prism
Lasers and Coherent Light Sources 11.1 Principles of Lasers 609

obtain N1 − N2  Nt /(1 + I/Is ), where Nt = N1 + N2 is


the total absorber population and Is ≡ hν/(2στ) is the
rber
Abso saturation intensity of the absorber. Since now the ab-
stic Diffracted sorption coefficient is α = σa (N1 − N2 ), from the last
Acou e two equations we obtain
wav beam
α0
Laser α= , (11.66)
2èB 1 + I/Is

Part C 11.1
beam
where α0 = Nt σa is the unsaturated absorption coef-
èB
ficient of the absorber. Equation (11.66) then shows
that, as the intracavity laser intensity I increases, the
losses introduced by the saturable absorber decrease
and the cavity Q correspondingly increases, i. e., Q-
Piezoelectric
RF voltage transducer
switching is achieved. The detailed dynamics underlying
the formation of a Q-switching pulse with the saturable-
Fig. 11.22 Schematic of an acoustooptic modulator used for absorber Q-switch, is however more involved than the
laser Q-switching (θB is the Bragg angle) one previously discussed. Here we just say that the
saturable absorber should have a low value of the sat-
beam propagating across such a grating (Fig. 11.22) thus uration intensity so that, when laser action starts, the
produces a diffracted beam and hence additional losses absorber is bleached earlier (i. e., at lower intensity)
in the cavity (low-Q condition). Maximum diffraction than the time when population inversion in the gain
efficiency is achieved when the incident light angle θB medium starts to decrease appreciably owing to stim-
satisfies the Bragg condition θB = λ/(2λa ), where λ ulated emission.
and λa are the optical and acoustical wavelengths, re- Typical absorbers used for passive Q-switching con-
spectively. The high-Q condition is simply obtained sist of dyes in an appropriate solvent; the main drawback
by switching off the transducer voltage. Acoustoop- of these absorbers is their photochemical degradation,
tic modulators have the advantages of introducing low i. e., poor chemical stability, and inadequate thermal
values of optical insertion losses and can be driven properties. Recently, the advent of solid-state absorbers
at high repetition rates (several kHz). Therefore they (notably absorbers based on chromium doped into vari-
are used mainly for repetitive Q-switching of low-gain ous crystalline hosts) are replacing dye absorbers, thus
CW-pumped lasers (e.g., Nd:YAG or Ar-ion lasers). avoiding the problem of degradation.

Saturable absorber Q-switching. The Q-switching Laser Mode-Locking: Dynamical Aspects


techniques discussed so far use active Q-switches, in Mode-locking is a laser operation regime in which many
the sense that they need an external control source. longitudinal modes of the cavity are simultaneously
A notable passive Q-switching technique, in which no forced to oscillate with a precise phase relation so that
external driving control is required, consists of placing the output laser beam shows a repetitive train of ultra-
a suitable saturable absorber inside the laser cav- short optical pulses [11.3, 5]. To achieve mode-locking
ity. This absorber is basically an unpumped two-level operation, a suitable device, which is usually referred
medium which absorbs at the laser wavelength with to as the mode locker, must be placed inside the cavity.
a comparatively low saturation intensity. Thus, due to For a given laser medium, the lower limit to the achiev-
the phenomenon of saturation, the absorption coeffi- able pulse duration ∆τp is set by the gain line width
cient of the absorber decreases as the intensity of the (∆τp  1/∆ν0 ), whereas the pulse repetition rate 1/τp
intracavity laser beam increases. To model this phe- is usually equal to the difference frequency between two
nomenon we write the rate equation for the absorber as consecutive longitudinal modes ∆ν (or an integer mul-
( dN2 / dt) = σa (N1 − N2 )I/(hν) − N2 /τ, where N2 and tiple of ∆ν, as for harmonic mode-locking). Therefore,
τ are the population and lifetime of the excited level 2, pulse duration, depending upon the gain line width, usu-
N1 is the population in the lower (ground) level 1, and ally ranges from about 1 ns, in gas lasers, down to 10 fs in
I = I(t) is the intracavity laser intensity. In CW opera- broad-bandwidth solid-state lasers. Pulse repetition rate
tion or if τ is short enough as compared to the changes depends, of course, upon the cavity length and usually
of I(t), we may assume that ( dN2 / dt) ≈ 0 and therefore ranges from about 100 MHz to a few GHz.
610 Part C Coherent and Incoherent Light Sources

Frequency-domain description. The basic principle of In a free-running laser, the phases ϕl do not have
laser mode-locking can be explained as follows. Let us a precise relation to each other; they may also fluctuate in
consider, for simplicity, a traveling-wave ring laser of time. The superposition of N modes with, e.g., the same
optical length L e , and assume that the separation of the amplitude Al = A0 but with randomly distributed phases
longitudinal cavity modes ∆ν = c/L e be smaller (usu- typically leads to a spiking signal |A(t)|2 made of a pe-
ally much smaller) than the gain line width ∆ν0 . In riodic sequence of irregular pulses (Fig. 11.24a), each
this case, even in the absence of the mode locker, the with duration approximately equal to ∆τp ≈ 1/∆νL ,
Part C 11.1

laser tends spontaneously to oscillate on several longi- where ∆νL = N∆ν is the oscillating bandwidth. Note
tudinal modes (free-running regime). Let νl = ν0 + l∆ν that, since the response time of a conventional photode-
be the frequency and El = Al exp(iϕl ) the complex am- tector is usually much longer than a few picoseconds,
plitude of the l-th oscillating longitudinal cavity mode, the complex temporal behavior shown in Fig. 11.24a is
where l is an integer number and l = 0 corresponds to the usually not resolved for free-running multimode lasers,
longitudinal mode closest to the center of the gainline instead its average value – proportional to N A20 – is
(Fig. 11.23). The electric field E(z, t) inside the laser monitored.
cavity is then given by the superposition of the oscillat- In a mode-locked laser, the role of the mode locker
ing longitudinal modes and can be written in the form is to lock the phases of oscillating modes in a precise
E(z, t) = A(t − z/c) exp[2πiν0 (t − z/c)], where z is the manner. The most common and interesting case is that
longitudinal coordinate measured along the perimetric of a mode locker that imposes a linear phase locking
axis of the ring and the envelope A(t ) is given by condition, i. e., ϕl = lϕ, where ϕ is a constant. In this
 case, one has:
A(t ) = Al exp(2πil∆νt + iϕl ) , (11.67) ∞

l A(t ) = Al exp(2πil∆νt ) , (11.68)
l=−∞
where t = t − z/c is a retarded time. Note that, owing to
the dependence of the field on t − z/c, the field distribu-
tion in the cavity is a traveling wave which propagates a) |E (t)|2
with the speed of light; therefore we may limit the dis- TR
cussion to the field behavior at a given reference plane
z = 0, e.g., at the output coupler of the laser. The output
laser power, averaged over the rapidly varying optical Äôp
cycle, will be then proportional to |A(t)|2 . Note that, if
the mode amplitudes Al and phases ϕl are constant or
slowly varying in time compared to the cavity round-trip
time τR = L e /c = 1/∆ν, the signal A(t) is basically pe- 0 0.5 1 1.5 2
riodic in time with a period equal to τR . However, the t /TR
specific form of the signal in one period depends on the b) |E (t")|2
precise distribution of the mode amplitudes Al and, most
ôp = TR ôp = TR
importantly, on their phases ϕl .

Äôp
Gain line

Äí0
–3 –2 –1 l = 0 1 2 3 0 0.5 1 1.5 2
t"/TR

Äí Fig. 11.24a,b Behavior of output power in a laser oscil-


ÄíL lating on many longitudinal modes with equal amplitude
(a) Free-running regime, corresponding to random phases
Fig. 11.23 Schematic of a laser oscillating on several longi- φl . (b) Mode-locking regime, corresponding to linear phase
tudinal modes in the frequency domain locking φl = lφ
Lasers and Coherent Light Sources 11.1 Principles of Lasers 611

where t is a translated time given by t = t + Time-domain description. The previous analysis of


ϕ/(2π∆ν). Usually, in a mode-locked laser the en- mode-locking is often referred to as the frequency-
velope of the mode amplitudes Al follows the shape domain description since the onset of the periodic pulse
of the gainline, i. e., Al is maximum at the center of train is viewed as due to the coherent superposition of
the gainline (l = 0) and decreases toward zero as |l| longitudinal modes of the laser cavity. A different de-
increases; for instance, for active mode-locking in a ho- scription of the mode-locking regime, complementary
mogeneously broadened medium, one can show that to the frequency-domain approach, is also possible in

Part C 11.1
Al follows a Gaussian distribution. However, to cal- the time domain. In fact, according to the results shown
culate the series in (11.68) simply, we assume that in Fig. 11.24b and since τR is the time for a round-trip,
Al = A0 = const. for |l| ≤ N and Al = 0 for |l| > N, a single pulse of duration ∆τp is circulating within the
i. e., we assume an odd number 2N + 1 of oscillating laser cavity (Fig. 11.25a). Note that the spatial extension
modes with the same amplitude. In this case one ob- of the pulse ∆z = c∆τp , according to (11.70) is given
tains in (11.68) a geometric progression which can be by ∆z = L e /(2N + 1) where L e is the length of the ring
calculated in a closed form, yielding perimeter. For a sufficiently large number (2N + 1) of os-
  cillating modes, ∆z is then much smaller than the cavity
sin (2N + 1)π∆νt
A(t ) = A0 . (11.69) length L e . The temporal periodicity of the output laser
sin(π∆νt ) beam then simply results from the successive transits
A plot of the squared amplitude of the electric field of the intracavity circulating pulse at the output mirror,
|A(t )|2 is reported in Fig. 11.24b. Note that a pulse which occur at intervals τp = L e /c equal to the cavity
train, at a repetition rate τp = 1/∆ν equal to the cavity transit time. According to this picture, we readily under-
round-trip time τR , is obtained. The squared ampli-
tude of the electric field at the peak pulse is given by a) Gain
(2N + 1)2 A20 , whereas the FWHM pulse duration ∆τp medium Output
is approximately given by beam
1 1 c
∆τp  = , (11.70)
(2N + 1)∆ν ∆νL
Pulse
where ∆νL = (2N + 1)∆ν is again the oscillating band- Mode
width. Therefore, for broad oscillating bandwidths, locker
phase locking among longitudinal modes leads to the
generation of short laser pulses with high peak power.
The physical limit to the maximum number of phase-
b) Gain Mode
locked modes that can be forced to oscillate is ultimately Pulse
medium locker
determined by the gain bandwidth of the active material, c
Output
i. e., ∆τp is longer than or equal to 1/∆ν0 . beam
In general, when the actual shape (e.g., Gaus-
sian) of the mode amplitudes Al is taken into
L
account, the overall field amplitude A(t ) can be
Gain medium
obtained approximately from (11.68) upon trans-
forming the sum  +∞over all modes into an integral, c) Mode
namely A(t )  −∞ A(l) exp(2πil∆νt ) dl. From this locker
last equation one then sees that the pulse amplitude c c c
Output
A(t ) is the Fourier transform of the spectral mode beam
envelope A(l). Therefore, in this case, i. e., under lin-
ear phase-locking conditions, the pulse amplitude is
2L/3 L/3
said to be transform limited. Note, however, that un-
Gain medium
der phase-locking conditions different from the linear
case (e.g., ϕl = ϕ1 l + ϕ2l 2 , as in so-called frequency Fig. 11.25a–c Schematic of the mode-locking regime in the
mode-locking) the mode-locked pulses are no longer time domain. (a) Mode-locking in a ring cavity. (b) Mode-
transform-limited, i. e., their temporal duration is larger locking in a linear cavity. (c) Harmonic mode-locking in
than that predicted by the Fourier limit. a linear cavity (harmonic order n = 3)
612 Part C Coherent and Incoherent Light Sources

stand that the mode-locking regime can be achieved by modulation (AM) mode locking], or a phase modulator,
placing a suitable fast shutter inside the cavity. In fact, which periodically varies the optical length of the res-
if an initially non-mode-locked beam is present within onator [frequency-modulation (FM) mode locking]. In
the cavity, its spatial amplitude distribution can be rep- lasers with upper-state lifetimes shorter than the cavity
resented as in Fig. 11.24a, with the time t replaced by round-trip time (e.g., dye lasers), active mode lock-
z/c. By periodically opening the shutter for a short time ing can also be achieved by periodic modulation of
interval (of the order ∆τp ) with period τp = L e /c, pos- the laser gain at a repetition rate equal to the longi-
Part C 11.1

sibly at the time when the most intense noisy pulse in tudinal mode separation ∆ν (synchronous pumping).
Fig. 11.24a reaches the shutter, then only this pulse will We limit here to describe the basic principle of AM
survive in the laser cavity, producing the mode-locking mode locking, since it is the most common among
condition of Fig. 11.24b. After a transient leading from the three mentioned techniques. In AM mode locking,
the temporal pattern of Fig. 11.24a to that of Fig. 11.24b, the mode locker is usually a Pockels-cell electroop-
the mode-locked pulse will consistently reproduce itself tic modulator for pulsed and high-gain lasers, or an
after each transit in the cavity. acoustooptic modulator for low-gain lasers. The elec-
It should be noted that all considerations made above trooptic or acoustooptic modulator sinusoidally varies
for a ring laser resonator apply mutatis mutandis to a lin- the cavity loss γ (t) at a given modulation frequency
ear (i. e., Fabry–Pérot) laser cavity. In this case, however, νm (Fig. 11.26). It is thus expected that the mode-
self-consistent propagation of the mode-locked pulse in locked pulse circulating inside the cavity (Fig. 11.25b)
one cavity round-trip requires that the shutter must be will pass through the modulator at the time t1 of the
placed close to one end mirror of the cavity (Fig. 11.25b). cycle where the cavity loss γ (t) is minimum. Since
Note that, if the shutter is placed at a distance L/2, L/3, the pulse propagating inside the cavity passes again
· · · , L/n from one end mirror and is opened at inter- through the modulator at times t2 = t1 + τR , t3 = t2 + τR ,
vals τR /2, τR /3, · · · , τR /n, where L is the cavity length, etc., where τR = 1/∆ν is the cavity round-trip time,
multiple pulses (precisely 2, 3, · · · , n pulses) may be a steady mode-locking regime can be reached provided
simultaneously generated and the repetition rate of the that the synchronization condition ∆ν = νm is satisfied.
pulse train is correspondingly increased by a factor of It should be noted that the steady-state pulse dura-
2, 3, · · · , n (see, e.g., Fig. 11.25c for the case n = 3). tion, ∆τp , is given by the inverse of the oscillation
Such a mode-locking regime is referred to as harmonic bandwidth, (2N + 1)∆ν, and, thus, it is ultimately es-
mode-locking. Harmonic mode-locking is typically em- tablished by the gain bandwidth ∆ν0 . However, the
ployed in active mode-locked fiber lasers to increase the finite bandwidth of the gain medium influences the
pulse repetition rate (≈ 1–40 GHz); owing to the rel- steady-state pulse duration in a quite different way
atively long cavity length (≈ 1–10 m), to reach high for homogeneous or inhomogeneous lines. For an in-
repetition rates harmonic orders n up to ≈ 1000 are homogeneously broadened line, and for a laser well
usually needed. above threshold, the oscillating bandwidth tends to
cover the whole gain bandwidth ∆ν0∗ even in the ab-
Mode-Locking Methods sence of AM modulation, and the main role of the
The methods to achieve mode-locking can generally be mode-locker is just to lock the phases of these os-
divided into two categories: cillating modes. The resulting temporal duration of
the mode-locked pulse is therefore given approxi-
1. Active mode locking, in which the mode-locker is
driven by an external source.
ã TR = 1/ím
2. Passive mode locking, in which the mode-locker is
not externally driven but exploits some nonlinear ã (t)
optical effect, such as the saturation of a saturable
absorber or the nonlinear change of the refractive
index in a Kerr medium.
|E (t)|2
Active mode locking. Active mode locking is usu-
ally achieved by placing, inside the laser cavity, either t1 t2 t3 t
an amplitude modulator, which produces a periodic
modulation in time of the cavity loss [amplitude- Fig. 11.26 Schematic of AM active mode locking
Lasers and Coherent Light Sources 11.1 Principles of Lasers 613

mately by
ã, g
0.44
∆τp  . (11.71) ã (t)
∆ν0∗
Conversely, for a homogeneously broadened gain
medium the number of longitudinal modes oscillating g
in the free-running regime is usually rather modest and I (t)

Part C 11.1
the role of the mode-locker is both to enlarge the oscil-
lating bandwidth of the laser (by power transfer from t
the central to lateral longitudinal modes) and to lock Fig. 11.27 Mode-locking with a fast saturable absorber
the phases of the oscillating modes. Under steady-state
conditions, band enlargement due to the modulator is loss experienced by a pulse crossing the absorber is
counteracted by band reduction due to the gain medium dependent on the instantaneous pulse intensity I(t),
and the pulse duration is given by [11.14] and decreases as the intensity increases. Thus, start-
0.45 ing from the random sequence of light bursts occurring
∆τp  √ . (11.72)
νm ∆ν0 in the unlocked case (Fig. 11.24a), the gain–loss bal-
As an example, we will consider a mode-locked Nd:YAG ance will favor the growth and stabilization of the noise
laser oscillating on its homogeneously broadened line at pulse with the highest intensity. The steady-state sit-
λ = 1064 nm. Assuming ∆ν0  126 GHz (T = 300 K), uation, occurring in this case, can be described with
a linear cavity of length L e = 1.5 m and an AM mode- the help of Fig. 11.27. Here, gain saturation drives the
locker placed close to one cavity mirror, the modulator gain g below the cavity losses γ (t) except at those in-
loss must be driven at a frequency νm = ∆ν = c/(2L e )  stants where, due to the arrival of the pulse I(t) at
100 MHz, and the expected mode-locked pulse duration, the saturable absorber, the losses are reduced due to
according to (11.72), is ∆τp  125 ps. absorber saturation. During the time intervals corre-
It should be noted that in AM mode-locked lasers sponding to the hatched regions in Fig. 11.27, the gain
(as well as in the other active mode locking techniques) is then larger than the instantaneous loss γ (t). A so-
even small detunings of the modulation frequency νm called window of net gain is thus produced, which
from the cavity axial mode separation ∆ν may result in tends to increase the peak of the pulse and decrease
the destruction of the mode-locking operation. In prac- its wings, i. e., it tends to narrow the pulse. This nar-
tice a detuning |νm − ∆ν|/νm of the order of ≈ 10−4 rowing is again counteracted by pulse broadening due
is enough to destroy mode-locking. To obtain stable to the finite amplifier bandwidth until a steady-state
AM mode-locking, active control of the cavity length pulse duration, whose duration again depends on the in-
is sometimes required, especially when relatively long verse of the gain bandwidth, is eventually reached. Good
cavities are employed (such as for AM mode-locked candidates for saturable absorbers must have a short re-
fiber lasers). laxation time τ (∼ a few picoseconds or shorter) and
a small saturation intensity, given by Is = hν/(2σa τ).
Passive mode-locking. There are two main types of Thus, very large values for the absorption cross section
passive mode-locking (ML): σa (≈ 10−16 cm2 or larger) are needed. Ideal absorbers
are therefore dye molecules (e.g., cyanine dyes) or,
1. Fast saturable-absorber ML, which uses the satura- even better, semiconductors. A particularly interest-
tion properties of a suitable absorber (e.g., a dye ing saturable-absorber geometry consists of integrating
or a semiconductor) with a very short upper-state a multiple-quantum-well absorber between two mirrors
lifetime; whose spacing is such that the resulting Fabry–Pérot
2. Kerr-lens mode-locking (KLM), which exploits the etalon operates in antiresonance. Such a device has
self-focusing property of a suitable transparent Kerr been convincingly proven to generate both picosecond
medium. and femtosecond laser pulses from several broadband
solid-state lasers.
Fast saturable-absorber ML [11.15]. Consider a sat-
urable absorber with a low saturation intensity and Kerr-lens mode-locking. This technique is based on
a relaxation time shorter than the duration of the mode- the use of a nonlinear loss element simply consist-
locked pulses. According to (11.66), the absorption ing of a nonlinear Kerr medium placed in front of
614 Part C Coherent and Incoherent Light Sources

an aperture (Fig. 11.28). The nonlinear medium shows,


via the optical Kerr effect, an intensity-dependent re- r Kerr Aperture
medium Low
fractive index n = n 0 + n 2 I, where n 0 is the linear intensity
refractive index of the medium, I is the local light
intensity and n 2 is a positive coefficient (for a self- w
focusing medium) which depends on the strength
of the nonlinearity (e.g., n 2  4.5 × 10−16 cm2 /W z
Part C 11.2

for fused quartz and n 2  3.45 × 10−16 cm2 /W for


sapphire). A light beam with, e.g., a transverse
Gaussian intensity distribution I(r) = Ip exp[−2(r/w)2 ] High
intensity
that crosses a thin slice of the Kerr medium of l
length l thus experiences a transversely varying phase
shift δϕ = 2πln 2 I(r)/λ = (2πln 2 /λ)Ip exp[−2(r/w)2 ]. Fig. 11.28 Schematic of a Kerr lens with an aperture used
Close to the beam center r = 0, one can write in KLM
δϕ ≈ (2πln 2 Ip /λ)[1 − 2(r/w)2 ], i. e., the thin medium
introduces a quadratic phase change of the field and mitted through the aperture. Therefore, the Kerr medium
thus acts, for n 2 > 0, as a positive lens (called a Kerr with the aperture, like a fast saturable absorber, intro-
lens) of dioptric power 1/ f = 4n 2lIp /(n 0 w2 ), which duces losses that decrease when the instantaneous pulse
increases as the beam intensity Ip increases. If an aper- intensity is increased, thus leading to mode-locking.
ture is placed at some suitable distance from the Kerr Note that, by appropriately controlling the cavity dis-
medium, a beam with higher intensity will be focused persion, the shortest mode-locked pulses (≈ 6 fs) have
tighter and a higher fraction of the beam will be trans- been achieved by this technique for Ti3+ :Al2 O3 lasers.

11.2 Solid-State Lasers


11.2.1 Basics crystals [11.28, 29] as tunable room-temperature lasers
has stimulated further research in transition-metal ions.
Solid-State Lasers Interesting new results have been obtained with the Cr4+
Based on Dielectric Insulators ion [11.30–33] and recently also with the divalent Cr2+
The demonstration of the ruby laser [11.16] ion [11.34].
(Cr3+ :Al2 O3 ) in 1960 led to a decade with the realization Nowadays, average and CW output powers for
of a number of crystalline and glass lasers. Especially Nd3+ - and Yb3+ -doped crystals in the kW range are
Nd:YAG [11.17], Nd-doped yttrium aluminum garnet commercially available. Fiber lasers reach output pow-
(Nd:Y3 Al5 O12 ), rapidly emerged as one of the most im- ers in the 100 W range with nearly diffraction-limited
portant crystalline dielectric lasers. The first glass laser beam quality.
was a fiber laser [11.18], which decades later led to Compact solid-state lasers in the visible spectral re-
the development of highly efficient Er-doped fiber am- gion (see for instance [11.35]) are of potential interest,
plifiers (EFDA) with important applications in optical especially for display and high-density optical data stor-
communications. age applications. Optical efficiencies of more than 20%
In the last two decades progress in the area of with respect to the pump power can be obtained in Nd
diode-pumped lasers has contributed very much to lasers by internal frequency doubling with nonlinear
a renaissance in the field of solid-state lasers. With crystals. An alternative approach enables the genera-
diode laser pumping it is possible to obtain higher tion of visible laser radiation by upconversion schemes,
efficiencies and to build rigid all-solid-state devices which incorporate energy transfer processes or two-
with simpler and more compact design. Besides Nd3+ step pump processes as ground-state and excited-state
various efficient diode-pumped rare-earth lasers have absorption.
been operated with Er3+ , Tm3+ , Ho3+ [11.19–21], In a most general sense lasers based on solids include
and Yb3+ [11.22, 23]. In addition, the successful op- both dielectric insulators and semiconductors as gain
eration of Cr3+ -doped [11.24–27] and Ti3+ -doped media. However, the development in the past yielded
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 615

a subdivision into two laser classes based on solids: can be determined according to Hund’s rule. Fig. 11.29
solid-state lasers (the topic of this chapter) and semi- shows the 4fn energy levels of rare-earth ions (Dieke
conductor lasers (Sect. 11.3). diagram [11.37]).
Nearly all modern, important solid-state lasers are Electric dipole transitions within the 4f-shell are par-
based on impurity-doped crystals or glasses. Typically, ity forbidden in the free ion. When doped in a solid,
the impurity ions have unfilled electronic shells. So far, acentric perturbations of the crystal field can however
only laser ions from the iron, rare-earth and actinide create admixtures of wave functions with opposite parity

Part C 11.2
group are known. The most important laser lines of these (for instance 4fn−1 5d1 states) yielding so-called forced
ions correspond to 4f–4f, 4f–5d, and 3d–3d transitions. electric dipole transitions. Due to the screening of the
In special cases the laser active ions can also be fully outer filled 5s2 and 5p6 orbitals, the crystal field per-
substituted into the lattice (stoichiometric laser mater- turbation is small and electron–phonon coupling is very
ials). It should be noted that in the past lattice defects weak. So, for rare-earth ions at acentric sites one ob-
also have been used as laser-active centers (color cen- serves electric-dipole zero-phonon transitions with very
ter lasers); these lasers are however not included in this weak vibronic sidebands. When doping occurs at cen-
chapter. tric sites, parity remains a good quantum number and all
4f–4f transitions remain electric dipole forbidden. The
Spectra of Rare-Earth magnetic-dipole emission cross sections are then very
and Transition-Metal Ions in Solids small and are not useful for laser applications.
4f–4f transitions in rare-earth ions. In the free rare- Further selection rules for electric dipole transitions
earth ion the electrostatic interaction between the 4f between 4fn states are:
electrons creates a splitting of the energy levels of the
4fn configuration into different L S terms. The resultant • ∆J ≤ 6; ∆S = 0, ∆L ≤ 6 (Russel–Saunders approx-
wave functions are characterized by the quantum num- imation)
bers L, S, M L , and M S . The electrostatic energy splitting • J = 0 ⇔ J = 0 is forbidden.
of the {2S+1} L terms is typically 104 cm−1 , and each level
is (2L + 1)(2S + 1)-fold degenerate with respect to M L 3d–3d transitions in transition-metal ions. The 3d
and M S . electrons of transition-metal ions are not shielded and
In addition, the energy levels are further split by experience a strong perturbation from the crystal field
spin–orbit coupling. If the energetic separation between of the surrounding ligand ions. Therefore, the energy-
different L S terms is large compared with the spin– level scheme and also the spectroscopic characteristics
orbit coupling energy there is only a small mixing of of a transition metal ion depend strongly on the strength
the L S terms. If this mixing is very small, the Russel– and the symmetry of the crystalline field originating
Saunders approximation holds and the wave functions from the surrounding ions. The energy-level schemes
are characterized by the quantum numbers L, S, J, M J of the transition-metal ions in crystalline hosts are de-
with a degeneration of (2J + 1). The typical splitting of scribed by so-called Tanabe–Sugano diagrams [11.38].
{2S+1} L terms is of the order of 1000 cm−1 . Although
J These diagrams are distinguished by the number of elec-
L S coupling is not strictly valid for rare-earth ions, it is trons within the 3d electron shell. In these diagrams the
usual to describe the 4f energy states with the Russel– energy levels of the transition-metal ion are presented as
Saunders approximation [11.36]. a function of the crystal field strength (for some exam-
The interaction of the 4f electrons with the crystal ples, see Sect. 11.2.3). For detailed reading appropriate
field, i. e., the electrostatic field of the surrounding lig- literature can be found in [11.36, 39–42].
ands, results in a Stark splitting of the free ion {2S+1} L J Due to the strong interaction with the surrounding
terms. This interaction can be treated as a perturbation of ions of the lattice, transition-metal ions mostly exhibit
the free ion levels. The crystal field splitting and the re- broadband emission because of the electron–phonon
maining degeneracy depend on the symmetry of the local coupling between the electronic 3d levels and lattice
crystal field. Lower symmetries increase the number of vibrations. As in the case of 4f–4f transitions, only
split levels. However, according to Kramers theorem an acentric perturbations can induce electric dipole transi-
odd number of electrons always yields at least twofold tions. Generally the spectra consist of a purely electronic
degeneracy. The Stark splitting is typically in the energy zero-phonon line with vibronic sidebands. In contrast
range of several 100 cm−1 . The ground state of a special to the situation in rare-earth ions, transition-metal ions
4fn configuration (the number of 4f electrons n = 1–14) at centric sites may also have reasonable transition
616 Part C Coherent and Incoherent Light Sources

Energy E (103 cm–1)


1S 6D 1S
40 0
U
7
9
2
2
U
T
38 3P
2
6I 1I
4G 3P 6
9
Part C 11.2

Z T 1
36 C 7
2 Y
2

O 2D 3P
N 5D 5 P 0
M 4 2
X S

34 R
6P L W 3L
R 7
2
3 V 3M 8 2K
Q 2 U
T Q 10 Q 13
P B 5 K 2
2
32 O
A 7
2 2P
S P 3
L J 2
R
N Q
30 M
P P
I O
H 5G
4D 3
1 2G
2 G 2 7
K 5D N
28 L 3
2
P
J
I 4
F
E
2
M N
3H
6 O
N
2
2 K 15 1D
M 9/2 2 2
U O 5 G'
H D
L 5 M
5L 4G
2P G C 10 3K 11
T N L
26 K 3
2
S
F B 5D
3
K
J
L
K
7 2
M 5G
E 4 2H
L I 9
R 5D 2
2D K D 3 K
24 5
2 Q
P I 4G
J 5
2P 11
I 1 H 2
2O 4F
3P H 5F 3
4I I 2
1
22 1I
2
4G
11 M
N G G 15
2
I
3K
6 H 5
2
F C 2 8 1G
6 2 4F H
1 G 3/2 9 9 G 4
2 E 5D F 2 2 4F
P D F 7
0 4G A 4 3 G 2
20 2G
3
2
L
K
C 7
2 2H
F 11
7 4F 2
E 2 5 S 1 F
S 2 4 4S
E E 3
4G 5S
18 2G
7
I
A 5
2
2 2

2 5 H
1D D 2 A 0
2 G
2H
11 5F
16 C
2
F 5 5F
5 4F
D 9
4F D 3F
2 2
B 9
2E 4
4S D 5S 6F 3
14 3
2
2 1
2
A 7 C 3
3 5I
2H
9 2 E 2 C 4
2 4
S 5 B 2 5
2
1
9 4
2A 1 B 2
D
12 3
R 2 7
2 B 5
6F C
O 11 6H 2F
1G 2 5 A 11
10 4
B
9
2 2 5
2
9 2 7
P 2 A 2 3H
A 6
5
11
8 R
5
5
2
W
2
9
2
3F 2 6H
R
4 4I V 8 S 15 13
2 Y 2
3 15 T 3
2 7F
6 2
U 1
2 0 X
11
2
4
7F 1
2 13 2 Y 7
3H W 7 V 2 6
6 13 3
4 2
W 11
2
5
13
X 6 4 Y 2
4
7 X 9
2 5 11 2
2 2
Y 5
3
5

Y 7
2 2

Z 1
0 Z Z Z Z

2 3 4 5 6 7 8 7 6 5 4 3 2
F5/2 H4 I9/2 I4 H5/2 F0 S7/2 F6 H15/2 I8 I15/2 H6 F7/2
n 1 2 3 4 5 6 7 8 9 10 11 12 13
Ce3+ Pr 3+ Nd3+ Pm3+ Sm3+ Eu3+ Gd3+ Tb3+ Dy3+ Ho3+ Er3+ Tm3+ Yb3+

Fig. 11.29 Energy level diagrams of trivalent rare earth ions of RE3+ in LaCl3 (“Dieke-diagram”) [11.37]
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 617

probabilities due to dynamical admixtures of wave func- energy-level structure of transition-metal ions is theo-
tions with different parity by acentric phonons. On the retically described by the ligand field theory and the
other hand, strong electron–phonon coupling can yield angular overlap model (AOM), see for instance [11.43].
higher temperature-dependent nonradiative decay rates
compared to 4f–4f transitions. The main interest in Spontaneous emission and emission cross section.
transition-metal ions is based on their broad tunability. The spontaneous emission is characterized by the Ein-
stein coefficient A. In an emission measurement, the

Part C 11.2
Interconfigurational 4f–5d transitions in rare-earth photon flux (the number of photons per area per time)
ions. Typically 4f↔5d interconfigurational transitions is usually measured. The normalization process with
of rare-earth ions are located in the ultraviolet spec- respect to the instrument response function can be per-
tral range. In some cases 4f↔5d transitions are also formed either with respect to photon flux or to the
observed in the visible spectral region. In contrast to spectral intensity distribution Iλ (λ) (energy per area per
3d↔3d and 4f↔4f transitions, 4f↔5d transitions are time). The relation between the spectral intensity dis-
−1
electric-dipole allowed, because they obey the parity tribution Iλ (λ), the Einstein coefficient A (A = τrad )
selection rule. Thus high transition probabilities and and the emission cross section σem (λ) is given by the
hence large absorption and emission cross sections Füchtbauer–Ladenburg equation [11.44]:
(≈ 10−18 –10−17 cm2 ) are observed.
λ5 Iλ (λ)A
Similar to 3d↔3d transitions strong electron– σem (λ) =  , (11.74)
phonon coupling yields broad absorption and emission 8πn 2 c Iλ (λ)λ dλ
spectra with spectral half-widths of more than where n is the refractive index and c is the speed of light.
1000 cm−1 . Therefore 4f↔5d interconfigurational tran- The emission cross sections can also be calculated
sitions are in principle suitable for the generation of from the absorption cross sections by the reciprocity
tunable laser oscillation. method
However, the difficulty in finding suitable pump  
Zl E zl − hc/λ
sources and often also excited-state absorption processes σem (λ) = σGSA (λ) exp ,
Zu kT
are major drawbacks with respect to the realization of
(11.75)
5d–4f lasers.
where Z l and Z u are the partition functions of the lower
Basic Spectroscopic Properties and upper energy levels, E zl is the energy of the zero-
and Laser Parameters phonon line of the corresponding transition, k is the
Ground-state absorption. The ground-state absorption Boltzmann constant, and T is the temperature.
of an ion is characterized by the absorption coefficient For Gaussian band shapes, which are often observed
α and the ground-state absorption cross section σGSA . for emission spectra of transition-metal ions, the Mc-
These values are derived using the Lambert–Beer law: Cumber formula can be used for the determination of
−n ion σ
GSA (λ)d , the peak emission cross section [11.45, 46]
I (λ) = I0 (λ) e−α(λ)d = I0 (λ) e 
(11.73) ln 2 A λ40
σem = , (11.76)
where I(λ) is the intensity transmitted through the crys- π 4πcn 2 ∆λ
tal at wavelength λ, I0 (λ) is the intensity in front of the where λ0 is the peak emission wavelength and ∆λ is the
crystal, n ion is the ion concentration, α(λ) is the absorp- full width at half-maximum (FWHM).
tion coefficient, σGSA (λ) is the absorption cross section,
and d is the crystal thickness. Excitation spectra. The excitation spectra allow the de-
The ground-state absorption spectrum contains in- termination of those absorption transitions, which yield
formation about the energy-level structure of the ion, a specific emission. These measurements are interesting
the cross sections σGSA (λ) and the oscillator strengths in the case of different absorbing and emitting centers
of the observed transitions. Note, that the calculation and also for finding energy transfer channels between
of cross sections needs a second independent measure- different optical active centers.
ment of the ion concentration, which is usually done by
X-ray microprobe analysis. The relation between the ab- Emission lifetime. The decay time of the metastable
sorption coefficient and the transition-matrix elements level of an ion in a crystal is usually measured after
can be derived using Fermi’s golden rule [11.36]. The excitation with a short pulse. The measured decay rate
618 Part C Coherent and Incoherent Light Sources

(measured as the number of transitions per unit time) knowledge of ESA processes is also very useful for
is the sum of radiative and nonradiative decay rates. In the determination of their influence on the efficiency of
general, the nonradiative decay of an ion can consist of a laser material. ESA may also inhibit gain and hence
intra-ionic multiphonon processes and intra-ionic nonra- laser action.
diative transfer processes (for details of energy transfer
processes see [11.36]). The equation for the decay is The laser aspect. In this section only the case of steady-
1 1 1 1 state conditions for laser oscillation will be discussed.
Part C 11.2

= A+ = + or For more details and for the case of pulsed excitation,


τ τnr τr τnr
see e.g. [11.49–52].
W = A + Wnr = Wr + Wnr , (11.77)
The efficiency of a laser system can be described
where τ, τr , and τnr are the total, radiative, and nonra- by the laser threshold Pthr and the slope efficiency
diative decay times, respectively, and W, Wr , and Wnr η = dPout / dPabs , where Pout and Pabs are the laser out-
are the total, radiative, and nonradiative decay rates, put power and the absorbed pump power, respectively.
respectively. Under the assumptions of only one metastable level (i. e.,
The determination of the Einstein coefficient A is not the upper laser level), ideal overlap between pump beam
an easy task, because in a simple decay measurement and resonator mode, homogeneous pump profile, low
the combined lifetime is always measured. An addi- mirror transmission and low passive losses as well as the
tional measurement of the emission quantum efficiency absence of excited-state absorption, the following equa-
ηQE would allow the determination of the radiative and tions hold for continuous-wave operation [11.49, 50]
nonradiative decay rate
hνp
τ Wr Wr Pthr =
ηQE = = = ηp σse (λl ) τ
τr W Wr + Wnr   V
τ τr τ × T + L + 2dσGSA (λl ) (n ion − n thr )
⇒ τr = and τnr = . (11.78) 2d
ηQE τr − τ
(3-level system) , (11.79)
However, a direct measurement of the quantum effi-
hνp V
ciency is difficult and usually contains a high error. Pthr = (T + L)
Another approach is the indirect determination of ηp σse (λl ) τ 2d
the quantum efficiency by analysis of the temperature (4-level system) , (11.80)
dependence of the emission lifetime. The two most com- λp T
monly used models are the simple Mott model of the η = ηp , (11.81)
λl T + L
activation energy [11.47] and the more-sophisticated
model of Struck and Fonger [11.48] using the so- where hνp is the energy of pump photon, ηp is the
called single-configurational-coordinate model, which pumping efficiency, i. e., the fraction of absorbed pump
describes in a simplified way the interaction between photons that are converted into excited ions in the upper
the electronic center and the vibrating crystalline envi- laser level, σse is the stimulated emission cross section,
ronment. τ is the lifetime of the upper laser level, T is the mir-
ror transmission, L is the passive losses, d is the length
Excited-state absorption (ESA). Measurements of the of the laser crystal, σgsa is the ground-state absorption
excited-state absorption (ESA) spectrum give further cross section, n is the concentration of laser ions, n thr
insight into the energy-level structure of an ion. In is the threshold inversion density, λp is the pump wave-
the ground state absorption measurements spin-allowed length, λl is the laser wavelength, and V is the pump
transitions are mainly observed and often spin-flip tran- volume.
sitions are hidden under these absorption bands. Thus In the following, several factors affecting the pump
the determination of the energy of these spin-flip transi- power threshold and the slope efficiency will be dis-
tions is often not possible. If the metastable level of the cussed.
ion has a different spin to the ground state (e.g., Cr3+
in strong crystal fields, Mn5+ , Fe6+ ), the ESA spec- Influence of the emission quantum efficiency ηQE .
trum reveals the energetic positions of these states with A quantum efficiency less than unity leads to lifetime
different spin. By using these data the crystal field pa- shortening and therefore to an increase in the laser
rameters can be determined with higher accuracy. The threshold, as can be seen from (11.79) and (11.80) after
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 619

replacing τ by ηqe τr level according to


   
hνp n 1 σESA λp
Pthr = (11.82) ηp = ηp,0 1−     ,
ηp σse (λl ) ηqe τr n 1 σESA λp + (n ion − n 1 ) σgsa λp
 
× T + L + 2dσgsa (λl ) (n ion − n thr ) (11.87)
V 1 where ηp,0 is the pumping efficiency without ESA, n ion is
× ∝ , (3-level) (11.83) the concentration of active ions, and n 1 is the population
2d ηqe

Part C 11.2
hνp V 1 density in the upper laser level. Therefore the pump
Pthr = (T + L) ∝ (4-level) . threshold is increased and the laser slope efficiency is
ηp ηqe σse τr 2d ηqe reduced according to (11.79, 80, 81).
(11.84) ESA on the laser wavelength also affects the laser
The quantum efficiency does not influence the slope threshold and the slope efficiency. The stimulated emis-
efficiency directly (11.81). However in practice a cor- sion cross section σse (λl ) in (11.79) and (11.80) is
responding, significant contribution of nonradiative replaced by σEFF (λl ) = σse (λl ) − σESA (λl ) and (11.81)
transitions increases the temperature in the pump vol- has to be extended [11.54]
ume and usually leads to a lower slope efficiency due λp σse (λl ) − σESA (λl ) T σEFF
η = ηp ∝ .
to further lifetime reduction and other problems such as λl σse (λl ) T +L σse
thermal lensing. (11.88)
If σESA (λl ) > σse (λl ) laser oscillation is not possi-
Influence of passive losses L. Passive losses in a laser ble.
system are due to imperfect optical components in the
laser resonator. This can be due to, e.g., stray centers 11.2.2 UV and Visible Rare-Earth Ion Lasers
and residual absorptions. Passive losses influence both
the threshold and the slope efficiency (11.79, 80, 81). In Lasers based on 5d ↔ 4f transitions of trivalent
a four-level system, the passive losses can be determined and divalent rare-earth ions
by the Findlay–Clay method [11.53]. For such an anal- In this section an overview of lasers oscillating in the
ysis, the laser threshold is measured as a function of ultraviolet and visible spectral range based on transi-
the output mirror transmission. The following equation tions of rare-earth ions is given. The first part deals with
holds: laser and possible laser systems based on interconfigu-
hνp V hνp V rational transitions, i. e., 4fn−1 5d → 4fn . In the second
Pthr = T+ L = mT + b , part, visible and UV lasers based on intraconfigurational
ηp σse τ 2d ηp σse τ 2d
(4fn →4fn ) transitions will be discussed. Both parts deal
(11.85)
with crystals as host materials. Finally, in the third part
hν an overview of fiber lasers in the visible spectral range
with slope m = ηp σsep τ 2d
V
and axis parameter b = m L.
is given.
From a linear fit to Pthr = Pthr (T ) both m and b are The 4f↔5d interconfigurational transitions of some
determined and thus the value of the passive losses L. divalent (RE2+ ) and trivalent (RE3+ ) rare-earth ions
An alternative way to determine the passive losses is to are located in the visible and ultraviolet spectral
rewrite (11.81) for a so-called Caird plot [11.54]: range. They are in principle suitable for the realiza-
1 λ L λ 1 tion of (tunable) laser oscillation. The transitions are
= + = m + b , (11.86) electric-dipole allowed and have high transition proba-
η ηp λp T ηp λp T
bilities and large absorption and emission cross sections
with slope m = ηpλλp L = b L. From a linear fit to η1 = of the order of 10−17 to 10−18 cm2 . Due to their

strong electron–phonon coupling, the observed absorp-
1 1
η T both m and b can be determined and thus the tion and emission transitions are broad (> 1000 cm−1 ).
value of the passive losses L. Difficulties with respect to laser operation are the non-
availability of efficient and simple excitation sources
Influence of excited-state absorption. ESA at the and the high probability of excited-state absorption and
pump wavelength reduces the number of pump pho- solarization (photoionization), e.g., Ce3+ :LiCaAlF6 and
tons converted into excited ions in the metastable laser Ce3+ :LiSrAlF6 depicted in Fig. 11.30.
620 Part C Coherent and Incoherent Light Sources

degenerated 2 T2 state and of a twofold orbital degener-


Conduction band of host ated 2 E level, from which the 2 T2 (2 E) state is at lower
energy in octahedral (cubic) symmetry. In Fig. 11.31 the
room-temperature absorption and emission spectrum of
óesa â ósol Ce3+ :LiYF4 is shown. In general, in the absorption spec-
3+ trum two to five broad bands are expected, depending
Ce
t2g (5d1) Impurity on the crystal field symmetry. In emission two bands
Part C 11.2

trap corresponding to the 5d→ 2 F5/2 and 5d→ 2 F7/2 tran-


óem
óabs sitions with an energetic separation of approximately
28 ns 0.3 s 2000 cm−1 are observed. The high cross sections of
Ce 3+ the electric-dipole- and spin-allowed 4f1 ↔5d1 transi-
2
F5/2 (4f1) tions correspond to an emission lifetime in the ns range.
Ce3+ -doped materials were therefore thoroughly inves-
tigated for application as tunable solid-state lasers and
Valence band of host
scintillators, see e.g., the overview articles by Coutts
et al. [11.57] and Dorenbos [11.58]. Laser oscillation
Fig. 11.30 Scheme of the energy levels in Ce3+ -doped was thus far achieved in YLiF4 [11.56], LuLiF4 [11.59],
LiCaAlF6 and LiSrAlF6 , where sABS , sEM , sESA , and sSOL , LiCaAlF6 [11.60], LiSrAlF6 [11.55, 61], LaF3 [11.62],
are the absorption, emission, ESA, and solarization cross and BaY2 F8 [11.63] crystals. The laser data are sum-
sections, respectively. From [11.55] marized in Table 11.2. For Ce3+ -doped materials the
main obstacle with respect to laser oscillation is excited-
In the following the trivalent and divalent rare- state absorption assigned to transitions to the conduction
earth ions exhibiting short-wavelength emission will band, e.g., as is the case for Ce3+ :YAG [11.64, 65]. For
be briefly discussed together with a summary of the Ce3+ -doped LiCaAlF6 and LiSrAlF6 the ESA transi-
obtained laser results. tion leads to a solarization, i. e., impurity traps with
long lifetimes are populated (Fig. 11.30). With the help
Ce3+ Lasers. The Ce3+ 4f1 ground-state configura- of an anti-solarent pump, these traps are depleted and
tion splits into the 2 F5/2 ground state and the 2 F7/2 higher efficiencies are obtained [11.66, 67].
excited-state multiplet with an energy separation of ≈
2000 cm−1 . The 5d excited configuration consists in an Pr3+ (4f 2 ). The energy-level scheme of Pr3+ is shown
ideal octahedral or cubic symmetry of a threefold orbital schematically in Fig. 11.32. Pr3+ has a 4f2 ground-state

Absorbance Fluorescence (arb.units) Output energy (mJ)


3 0.3

2.5 0.25
5d

2 0.2
Fluorescence Slope 47 %
1.5 0.15
} 4f

1 Absorption 0.1

0.5 0.05

0 0
200 250 300 350 0 0.1 0.2 0.3 0.4 0.5 0.6 0.7
Wavelength (nm) Absorbed input energy (mJ)

Fig. 11.31 Left: Absorption (solid line) and emission (dotted line) spectra of Ce3+ :LiYF4 . The inset shows the schematic
energy level diagram. From [11.56]. Right: Input-output characteristic of a 2% Ce3+ , 2% Na:LiSrAlF6
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 621

Table 11.2 Overview of lasers based on the 5d→4f transitions of trivalent and divalent rare-earth ions (CVL: copper vapor laser,
RS: Raman-shifted)
Laser material λlas (nm) Eout , Pout ηsl Tuning range (nm) Pump source Ref.
Ce3+ :LiYF4 325.5 KrF, 249 nm [11.56]
Ce3+ :LiLuF4 309 27 mJ 17% 307.8– 311.7 & 323.5– 326.5 KrF, 249 nm [11.75]
2.1 mJ 55% 307.6– 313.5 & 324 –328.5 Ce:LiSAF, 290 nm [11.76, 77]
309 77 µJ 309.5– 312.3 & 324.5– 327.7 Nd:YAG, 5ω(213 nm) [11.78]

Part C 11.2
309.5 300 mW 38% 305.5– 316 & 323–331 CVL, 2ω(289 nm), 7 kHz [11.79]
309 67 mW 62% RS Nd:YAG, 4ω(289 nm), [11.80]
10 kHz
Ce3+ :LiCaAlF6 290 21% Nd:YAG, 4ω(266 nm) [11.55]
289 60 mJ 26% Nd:YAG, 4ω(266 nm) [11.81]
289 30 mJ 39% 284–294 Nd:YAG, 4ω(266 nm) [11.82]
289 550 mW 27% 280–311 Nd:YAG, 4ω(266 nm), 1 kHz [11.83]
288.5 530 mW 32% 280.5– 316 2ω CVL, 271 nm, 7 kHz [11.79]
289 0.53 µJ 31% 283–314 Nd:YVO4 , 4ω(266 nm), 1 kHz [11.84]
289 230 µJ 49% 280–317 Nd:YLiF4 , 4ω(263.3 nm), [11.85]
0.1–4.3 kHz
Ce3+ :LiSrAlF6 290 29% Nd:YAG, 4ω(266 nm) [11.55]
290 47% Nd:YAG, 4ω(266 nm) [11.66]
+ 2ω(532 nm)
281–315 nm Nd:YAG, 4ω(266 nm) [11.86]
Ce3+ :LaF3 286 ≈ 5 µJ KrF, 249 nm [11.62]
Ce3+ :BaY2 F8 345 XeCl, 308 nm [11.63]
Nd3+ :LaF3 172 Kr, 146 nm [11.87, 88]
F2 Laser, 157 nm [11.89, 90]
Sm2+ :CaF2 708.5 708.5–745 nm (20–210 K) Xe flash lamp [11.91, 92]
(20 K)

configuration. In this configuration 91 energy levels Other RE3+ ions. The lowest 4fn−1 5d1 energy levels for
exist, distributed over 11 manifolds, from which the ions from Nd3+ to Yb3+ are at even higher energies
3 H level is the ground state and 1 S is the highest and therefore in the vacuum ultraviolet (VUV) spec-
4 0
level at approximately 46 500 cm−1 . In the 4f1 5d1 con- tral region. Thus the corresponding transitions are not
figuration, 140 energy levels exist. Depending on the easy to access spectroscopically. A systematic study and
crystal field strength and splitting, either the lowest detailed analysis of the VUV spectroscopy of trivalent
4f1 5d1 level or the 1 S0 state is lower in energy. Thus rare-earth ions were performed by Wegh et al. [11.93].
after UV excitation, emission occurs either from the The exploitation of these VUV transitions for laser os-
4f1 5d1 level as a 4f1 5d1 →4f2 transition or from the 1 S0 cillation still requires much experimental efforts. Laser
level as a 4f2 →4f2 transition. In any case, the emis- oscillation on a 5d→4f transition besides for Ce3+ has
sion spectrum consists of several bands, because several thus far only been realized with Nd3+ :LaF3 at 172 nm
4f2 terminal levels exist. Spectroscopic investigations with a Kr2 laser at 146 nm as the pump source [11.87].
of the 4f↔5d transitions have so far been carried out
for a number of materials, e.g., Y3 Al5 O12 [11.68, 69], Divalent rare-earth ions. Rare-earth ions have a strong
YAlO3 [11.68, 70, 71], CaF2 , LiYF4 [11.71–73], and tendency to be incorporated into crystals in the trivalent
K5 PrLi2 F10 [11.71]. Thus far laser oscillation based state. In order to obtain the divalent state, the RE3+ ion
on the 4f1 5d1 →4f2 or on the 1 S0 →4f2 emission of needs to be reduced. Eu2+ , Yb2+ , Sm2+ and, with some
Pr3+ has not achieved. The main reason seems to be limitations, Tm2+ can already be obtained in significant
excited-state absorption into the conduction band, e.g., amounts during crystal growth by using suitable lattices
for YLiF4 [11.73], and into higher-lying 4f1 5d1 levels, containing divalent cation sites, appropriate codopants,
e.g., for Y3 Al5 O12 [11.74]. and a reducing growth atmosphere. The other RE2+ ions
622 Part C Coherent and Incoherent Light Sources

a) E (×1000 cm–1) b) E (×1000 cm–1)

Pr3+: LiYF4 Pr3+: YF3


90 90

80 80
Part C 11.2

70 70
t2g t2g
60 4f5d 60 4f5d
eg eg
50 50
1 1
S0 S0
Excitation
40 Excitation 40

30 30 Emission
1
Emission S 0 ® 1I 6
3
P2,1,0, 1I 6 3
P2,1,0, 1I 6
20 20
1
1
D2 D2
1
10 1
G4 10 G4
3
F4,3,2
3
F4,3,2 ×4
3 3
0 H6,5,4 0 H6,5,4

Fig. 11.32a,b Energy-level schemes of Pr3+ (a) Pr3+ :LiYF4 , E(4f 1 5d1 ) < E(1 S0 ), (b) Pr3+ :YF3 , E(4f 1 5d1 ) > E(1 S0 ).
(After [11.94])

are rather difficult to obtain in crystals; usually special Eu2+ (4f7 ). The 4f7 energy-level scheme of Eu2+ is
growth conditions as well as pre- and post-treatments spectroscopically similar to that of Gd3+ (Fig. 11.29).
are necessary, e.g., the use of sealed Ta ampoules dur- A large energy gap between the 8 S7/2 ground state and
ing crystal growth, pre-synthesis of REF2 and RECl2 , the 6 P7/2 first excited state exists. Depending on the
electron-beam irradiation etc. crystal field strength, the lowest 4f6 5d1 energy level is
5d→4f transitions are expected to occur for systems located above or below the 6 P7/2 level. Therefore, either
in which the 4fn−1 5d level is energetically located within narrow line emission due to the 6 P7/2 → 8 S7/2 transi-
a large energy gap between 4fn multiplets. These ions tion in the UV region or broadband emission due to the
are Sm2+ , Eu2+ , Tm2+ , and Yb2+ . 4f6 5d1 → 8 S7/2 transition in the blue to yellow spectral
range occurs. Laser oscillation based on a 4f6 5d1 →4f7
Sm2+ (4f6 ). The 4f6 energy-level scheme of Sm2+ is transition of Eu2+ has not been realized thus far due to
spectroscopically similar to that of Eu3+ (Fig. 11.29). excited-state absorption from the lowest 4f6 5d1 level to
For most crystals, Sm2+ emission occurs as a 4f6 →4f6 the conduction band and to high-lying 4f7 levels [11.96].
transition from the metastable 5 D0 level, which is located
at about 15 000 cm−1 . In CaF2 , the lowest 4f5 5d1 level Tm2+ (4f13 ). The 4f13 energy-level scheme of Tm2+ is
is located just below the 5 D0 level and broadband emis- spectroscopically similar to that of Yb3+ (Fig. 11.29).
sion occurs. Laser oscillation based on a 4f5 5d1 →4f6 Laser oscillation of Tm2+ was realized in CaF2 on the
transition was realized with Sm2+ :CaF2 [11.91,92]. The 5/2 → F7/2 transition at 1116 nm at temperatures be-
2F 2

laser wavelength is 708.5 nm at 20 K and increases with low 27 K [11.97,98] (Table 11.9). Laser oscillation based
temperature to 745 nm at 210 K, which is the highest op- on the 4f12 5d1 → 4f13 transition has not been obtained
eration temperature of the Sm2+ :CaF2 laser. This laser thus far. However, Tm2+ is an interesting candidate for
is affected by excited-state absorption assigned to tran- laser oscillation on a 4f12 5d1 → 4f13 transition, because
sitions to the conduction band and to high-lying 4f6 there are no high-lying 4f13 energy levels, which could
levels [11.95, 96]. interfere with the 4f12 5d1 energy levels and thus act as
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 623

possible terminal levels for excited-state absorption tran-


sitions or quenching processes. The transition between E (103 cm–1)
the lowest 4f12 5d1 level and the ground state is parity » 720 nm
30 » 700 nm » 910 nm
allowed, but spin forbidden. Thus the emission cross » 640 nm » 470 nm
» 600 nm » 530 nm
sections are expected to be about one to two orders of » 540 nm » 880 nm
» 490 nm » 630 nm
magnitude smaller compared to, e.g., those of the 5d→4f 3
1
I6 P2
transitions of Ce3+ . The Tm2+ → Tm3+ conversion ob- 3 3
P1
20 P0

Part C 11.2
served under UV/VIS lamp excitation [11.98] indicates
the strong tendency of the Tm ion towards the triva- 1
D2
lent state and has to be considered as a possible major
drawback for laser applications.
10 1
G4
3
Yb2+ (4f14 ). The ground-state configuration of the Yb2+ F4 3
F4
ion is 4f14 . This completely filled shell leads to a 1 S0 3
H2 3
H6
ground state of the free ion and other 4f14 levels 3
H5
3
do not exist. In an octahedral crystal field, this state 0 H4
transforms like the 1 A1 irreducible representation. The
excited 4f13 5d1 configuration consists in total of 140 Fig. 11.33 Energy-level scheme of the Pr3+ ion. The ob-
energy levels. The 4f13 5d level splits in a highly sym- served laser transitions in the visible spectral range are
metric crystal field into a threefold degenerated T2 indicated by arrows
and a twofold degenerated E level. The 4f13 elec-
trons can be considered as a Yb3+ -ion configuration ions. Laser oscillation has been realized under flashlamp
with the two manifolds 2 F7/2 and 2 F5/2 separated by pumping, direct laser pumping into the upper laser level
about ∆E 4 f ≈ 10 000 cm−1 . The spin of the 5d elec- or higher-lying energy levels and under upconversion
tron can either be parallel or antiparallel to that of pumping.
the 4f13 core, thus the whole energy-level scheme
exists for singlet and for triplet states, from which, Pr3+ lasers. The Pr3+ ion is a very interesting and
according to Hunds’ rule, the triplet states are ener- promising ion for obtaining efficient visible laser os-
getically lower. Note furthermore that for the Yb2+ cillation. Its energy-level scheme is shown in Fig. 11.33.
free ion the 6s level is energetically lower than the
5d level. Therefore it might be the case that in
some materials the 4f13 6s level is also the lowest óem (10–19 cm2)
excited state. This would lead to a parity- and spin- 4
E II a 3
forbidden transition requiring ∆L = 3 and ∆S = 1. The P 0 ® 3H 6
3
emission spectra of Yb2+ -doped materials consists of 2 P 0 ® 3F 4
a broad band (≈ 6000 cm−1 ) with the peak emission
3 3
P0 ® H 4 3
3 3
P0 ® F 2 3 3
P0 ® F 3
P 0 ® 3H 5
wavelength strongly dependent on the host material
0
(λpeak ≈ 390–575 nm) [11.99–103]. Laser oscillation E II b
has not been obtained thus far. The main reason is 5
3
P 1 ® 3H 4
excited-state absorption. In Yb2+ :MgF2 strong ESA 3
P 1 ® 3F 2
3
P 1 ® 3F 4
3 3 3 3
transitions in the whole spectral range of absorption P1 ® H 5 P1 ® H 6 3
P 1 ® 3F 3
and emission are observed, preventing laser oscillation. 0
The ESA cross section is about one order of magnitude E II c
larger than the absorption cross section and three orders 5
of magnitude larger than the stimulated emission cross
section [11.102, 103].
0
Lasers based on 4f ↔ 4f transitions of trivalent 500 550 600 650 700 750
Wavelength ë (nm)
and divalent rare-earth ions
This section deals with UV and visible lasers based on Fig. 11.34 Emission spectra of Pr3+ :BaY2 F8 at room temperature
the 4f↔4f transitions of trivalent and divalent rare-earth for different polarizations
624 Part C Coherent and Incoherent Light Sources

Laser transitions in the visible spectral range occur from characterization of a Pr3+ -doped laser material. For
the 3 P0 and the thermally populated 3 P1 and 3 P2 levels. Pr3+ :LiYF4 , laser oscillation on several transitions
In Fig. 11.34 the emission spectrum of the Pr3+ :BaY2 F8 has been obtained with slope efficiencies up to
as an example is shown. The peak cross sections are in ≈ 26% and output powers up to ≈ 270 mW [11.106]
the range of ≈ 1 to 5 × 10−19 cm2 and thus comparable (Fig. 11.36). However, the wavelength match be-
to the values of the Nd3+ 4 F3/2 → 4 I11/2 transition. The tween the Ar+ pump and Pr3+ absorption is bad
highest cross sections are in the orange and red spectral (Fig. 11.35). Furthermore Ar+ -ion laser pumping
Part C 11.2

range, therefore the most efficient lasers are expected itself is very inefficient, therefore the overall ef-
there. The first Pr3+ laser (λ = 1047 nm) was realized ficiency of a gas-laser-pumped Pr3+ laser is very
in CaWO4 as early as 1962 by Yariv et al. [11.104]. low.
Since then, laser oscillation has been obtained in more 2. Pumping with a frequency-doubled Nd3+ laser op-
than 20 materials on several transitions and under differ- erating on the 4 F3/2 → 4 I9/2 ground-state transition.
ent pumping conditions, see e.g., the review article by These ground-state lasers operate, depending on the
Kaminskii [11.105]. The major drawback of Pr3+ lasers host material, between 910 nm and 960 nm, i. e.,
is their excitation; see the discussion in section on Pr3+ the frequency doubling yields wavelengths between
laser. 455 nm and 480 nm. A Pr3+ laser directly pumped by
a frequency-doubled Nd3+ :YAG ground-state laser
Directly pumped Pr3+ lasers. In Fig. 11.35 the absorp- operating at 473 nm has been successfully demon-
tion spectrum of Pr3+ :BaY2 F8 for the spectral range strated by Heumann et al. [11.107]. Pr3+ laser
between 420 nm and 500 nm is shown. Direct pumping oscillation occurred at 639.5 nm on the 3 P0 → 3 F2
of the 3 P0 upper laser level is possible for several wave- transition with an output power of nearly 100 mW
lengths in the blue spectral range corresponding to the and a slope efficiency of 12%. Also for frequency-
3 H → 3 P , 3 P , 3 P , and 1 I transitions. In principle doubled Nd3+ ground-state lasers the match between
4 2 1 0 6
the following pumping schemes for direct excitation are the pump and absorption wavelength is crucial.
possible:
Pout (mW)
1. Ar+ -ion laser pumping. Ar+ -ion lasers offer the 200
possibility of continuous-wave pumping with a high- ë = 522 nm
quality pump beam. Therefore it allows the 150 T = 3.7 %, ç = 14.5 %
T = 3.4 %, ç = 3.8 %
100 T < 0.1 %, ç = 0.8 %
óabs (10–19 cm2)
6 50
3+ 3+
Pr , Yb : BaY2F8
300K, E II c 3 0
H 4 ® 3P 0
5 300 ë = 639.5 nm
Ar+, Nd: YAG SHG
T = 0.7 %, ç = 25.9 %
4 200
T = 12.8 %, ç = 20.4 %
Laserdiode Ar+ Ar+ Ar+ Ar+ Ar+
100
3 3
H 4 ® 3P 2
0
2 ë = 907.4 nm
3
H 4 ® 3P 1, 1I 6 20 T = 2 %, ç = 7.3 %
1
10
0
420 440 460 480 500 0
Wavelength (nm) 0 0.2 0.4 0.6 0.8 1 1.2
Pabs (mW)
Fig. 11.35 Absorption cross section spectrum of Pr3+ ,
Yb3+ :BaY2 F8 at room temperature. The relevant transi- Fig. 11.36 Input–output diagram of the CW Pr3+ :LiYF4
tions are assigned. The possible pump laser wavelengths laser at different laser wavelengths pumped by an Ar+ -ion
are also shown laser at 457.9 nm. (After [11.106])
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 625

3. Frequency-doubled optically pumped semiconduc- Table 11.3 lists Pr3+ lasers operating in the visible
tor lasers (OPS). These lasers are commercially spectral range under direct excitation. In Table 11.4 an
available with powers up to 200 mW [11.108]. In overview of the room-temperature laser data for visible
principle, the laser wavelength is adjustable (by Pr3+ lasers is given.
choosing the material parameters of the semiconduc-
tor) and can be tuned to match the absorption line Upconversion pumped Pr3+ lasers. Because of the dif-
of the Pr3+ ion. Output powers of approximately ficulties of direct excitation, other pumping schemes

Part C 11.2
35 mW with slope efficiencies of approximately using upconversion processes are under investigation
30% have been obtained [11.109]. Furthermore, for Pr3+ lasers. Upconversion describes a process in
Richter et al. used an OPS operating at 480 nm as which the photon energy of the excitation light (pump
a direct pump source [11.110]. A slope efficiency light) is converted via interaction with the active ions
of 40% and a maximum output power of 75 mW inside the optical material into higher-energy pho-
were obtained for Pr3+ :YLiF4 . For Pr3+ :BaY2 F8 , tons [11.113–116]. For Pr3+ with its high-lying energy
the corresponding data are 30% and 51 mW. It is levels upconversion is a suitable way to obtain visible
worth noting that intracavity frequency doubling laser oscillation under infrared pumping. Especially the
leads to continuous-wave UV radiation of about photon-avalanche pumping scheme, which is a com-
19 mW for Pr3+ :YLiF4 and Pr3+ :BaY2 F8 . Due to bination of different upconversion and energy transfer
the multi-wavelength operation of Pr3+ lasers, UV processes, has been efficiently exploited for the Pr,Yb
generation at 360 nm, 303 nm and even 261 nm codoped system. For crystals the Ti:Al2 O3 laser is
seems possible. These pump lasers are still expen- mainly used as the excitation source, but investigations
sive; however power scalability of OPS lasers can be are being performed on the use of commercially avail-
expected making these pump sources very attractive able laser diodes. In fibers, efficient laser operation has
for Pr3+ . already been achieved under laser-diode pumping (see
4. Blue and UV GaN laser diodes. These diodes operate page 633, Visible fiber lasers).
thus far in the spectral region below 450 nm and with The principle scheme of the photon-avalanche pro-
output powers in the mW range. Recently, Richter cess is shown in Fig. 11.37. A weak ground-state
et al. obtained laser oscillation at room temperature absorption yields the excitation of a few ions into the
with Pr3+ :YLiF4 under pumping with a 442 nm GaN intermediate (reservoir) level. The strong ESA process
laser diode [11.35]. The Pr3+ laser emits 1.8 mW efficiently brings these ions to the emitting level. An
at 639.7 nm. The threshold pump power and slope effective feedback mechanism for the reservoir level
efficiency were 5.5 mW and 24%, respectively. If the (in our system a cross-relaxation process) is necessary,
development of these diodes towards higher output which couples the emitting level, the reservoir level and
powers proceeds, laser diodes will certainly be one the ground-state level. After these two steps there are
of the best choices for the direct pumping of Pr3+ two ions in the reservoir level. This cycle repeats and
lasers. thus the population of the emitting (upper laser) level
5. Flashlamp pumping [11.111]. Under flashlamp exci- increases like an avalanche. If the threshold population
tation only a small fraction of the emitted radiation is reached, the laser oscillation on any transition from the
of the lamp can be used for the excitation of the upper laser level may start. The general characteristics
Pr3+ 3 P0 level, because of the narrow line width are described in detail in [11.113, 114, 117–119]; here
of the Pr3+ absorption lines and of the small spec- only the main points are given for the example of Pr3+ ,
tral range of these lines. Output energies up to Yb3+ :BaY2 F8 [11.120, 121]. The pump-power depen-
87 mJ and slope efficiencies of 0.3% have been dence of the emission intensity exhibits a threshold-like
obtained [11.111]. behavior. At this threshold, the slope increases sig-
6. Dye-laser pumping. The pump laser wavelength is nificantly. A second characteristic of the avalanche
tunable and thus can be adjusted to match the absorp- mechanism is the temporal S-shaped evolution of the
tion lines of the Pr3+ ion. Therefore, the obtained upconverted emission (Fig. 11.38).
lasers exhibit a high efficiency. For Pr3+ :LiGdF4 The photon-avalanche process has already been ob-
lasers, oscillation on several wavelengths and tran- served in a variety of materials, see e.g. [11.113, 114].
sitions with slope efficiencies up to 37% have been However, laser oscillation has only been obtained in
reported [11.112]. However, dye lasers are limited a few materials, see Table 11.5 for Pr3+ systems and
in their practical use. Table 11.6 for other rare-earth-ion-doped systems. The
626 Part C Coherent and Incoherent Light Sources

Table 11.3 Pr3+ lasers in the visible spectral range under direct excitation (bold: laser oscillation on some transitions
obtained at room temperature)
Crystal Transition Wavelength (nm) Ref.
LiYF4 3 P →3 H 479.0 [11.35, 106, 107, 110, 111, 122–126]
0 4
3 P →3 H 522.0
1 5
3 P →3 H 537.8, 545.0
0 5
Part C 11.2

3 P →3 H 604.4, 607.2, 609.2, 613.0


0 6
3 P →3 F 615.8, 618, 620.1
1 2
3 P →3 F 638.8, 639.5, 644.4
0 2
3 P →3 F 670.3
1 3
3 P →3 F 695.4, 697.7, 705.5
0 3
3 P →3 F 699.4
1 4
1 I →3 F 708.2
6 4
3 P →3 F 719.5, 720.9, 722.2
0 4
LiLuF4 3 P →3 H 538 [11.127, 128]
0 5
3 P →3 H 604.2, 607.1
0 6
3 P →3 F 639.9, 640.1
0 2
3 P →3 F 695.8, 697.7
0 3
3 P →3 F 719.2, 721.5
0 4
LiGdF4 3 P →3 H 522 [11.106, 112]
1 5
3 P →3 H 545
0 5
3 P →3 H 604.5, 607
0 6
3 P →3 F 639
0 2
3 P →3 F 697
0 3
3 P →3 F 720
0 4
KYF4 3 P →3 F 642.5 [11.106, 112]
0 2
BaY2 F8 3 P →3 H 607.1 [11.110, 125, 129–131]
0 6
3 P →3 F 638.8
0 2
3 P →3 F 693.5–693.8
0 3
3 P →3 F 719.1
0 4
LaF3 3 P →3 H 598.5, 600.1 [11.132–135]
0 6
3 P →3 F 719.4, 719.8
0 4
PrF3 3 P →3 H 598.4 [11.136]
0 6
LaCl3 3 P →3 H 489.2 [11.137–139]
0 4
3 P →3 H 529.8
1 5
3 P →3 H 616.4, 619.0
0 6
3 P →3 F 645.1
0 2
PrCl3 3 P →3 H 489.2 [11.137, 140]
0 4
3 P →3 H 529.8, 531
1 5
3 P →3 H 617, 620, 622
0 6
3 P →3 F 645.2, 647
0 2
LaBr3 3 P →3 H 532.0 [11.140]
1 5
3 P →3 H 621.0
0 6
3 P →3 F 632.0
2 3
3 P →3 F 647.0
0 2
PrBr3 3 P →3 H 622 [11.137, 140]
0 6
3 P →3 F 645.1, 649
0 2
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 627

Table 11.3 (continued)


Crystal Transition Wavelength (nm) Ref.
Y3 Al5 O12 3 P →3 H 487.2 [11.141, 142]
0 4
3 P →3 H 616
0 6
3 P →3 F 747
0 4
YAlO3 3 P →3 H 613.9, 621.3, 621.6 [11.143–147]
0 6
3 P →3 F 662

Part C 11.2
0 2
3 P →3 F 719.5, 719.7, 722
0 3
3 P →3 F 746.9
0 4
1 D →3 F 743.7, 753.7
2 3
LuAlO3 3 P →3 H 615.5 [11.144, 145, 147]
0 6
3 P →3 F 722.0
0 3
3 P →3 F 749.6
0 4
SrLaGa3 O7 3 P →3 H 488 [11.148]
0 4
3 P →3 F 645
0 2
CaWO4 3 P →3 F 649.7 [11.149]
0 2
Ca(NbO3 )2 3 P →3 H 610.5 [11.149]
0 6
LiPrP4 O14 3 P →3 H 604.8, 608.5 [11.150]
0 6
3 P →3 F 639.6
0 2
3 P →3 F 720.4
0 4
LaP5 O14 3 P →3 F 637 [11.151]
0 2
3 P →3 F 717
0 4
PrP5 O14 3 P →3 F 637.4 [11.152–154]
0 2
LaP5 O14 3 P →3 F 637.0 [11.151]
0 2

Table 11.4 Overview of room temperature laser data of directly pumped Pr3+ lasers in the visible spectral range
Host Transition λlaser (nm) Pump Pthr /Ethr Pout /Eout η (%) Ref.
LiYF4 3P
1 →3 H5 522.0 457.9 nm 163 mW 144 mW 14.5 [11.106]
3P
0 →3 H5 545.0 CW, Ar+ -ion laser 19 mW
3P
0 →3 H6 607 110 mW 7 mW 1.2
3P
0 →3 F2 639.5 8 mW 266 mW 25.9
3P
0 →3 F3 697 105 mW 71 mW 10.3
3P
0 →3 F4 720 98 mW 40 mW 7.2
3P
0 →1 G4 907.4 280 mW 23 mW 7.3
LiYF4 3P
0 →3 F2 639.5 473 nm CW, SHG Nd:YAG 40 mW ≈ 100 mW 12 [11.107]
LiYF4 3P
0 →3 H6 613 476 nm CW, Ar+ − ionlaser 45 mW ≈ 400 fs (ML) [11.124]
LiYF4 3P
0 →3 F2 639.5 442 nm CW, GaN laser diode 5.5 mW ≈ 1.8 mW 24 [11.35]
LiYF4 3P
0 →3 F2 639.5 480 nm CW OPS 37 mW 72 mW 40 [11.110]
LiYF4 3P
0 →3 F2 639.5 Xe flashlamp (60 µs) ≈ 7J 87 mJ ≈ 0.3 [11.111]
LiGdF4 3P
1 →3 H5 522 468 nm 197 µJ 83 µJ 27 [11.112]
3P
0 →3 H5 545 pulsed dye laser 49 µJ 2 µJ
3P
0 →3 H6 604.5 144 µJ 32 µJ 37
3P
0 →3 H6 607 50 µJ 2 µJ
3P
0 →3 F2 639 4 µJ 98 µJ 32
3P
0 →3 F3 697 73 µJ 31 µJ 26
3P
0 →3 F4 720 6 µJ 80 µJ 35
KYF4 3P
0 →3 F2 642.5 457.9 nm CW, Ar+ -ion laser 15 mW [11.106]
KYF4 3P
0 →3 F2 642.5 465 nm pulsed dye laser [11.112]
YAlO3 3P
0 →3 F4 746.9 476.5 nm CW, Ar+ -ion laser 25 mW 130 mW 24.6 [11.146, 155]
628 Part C Coherent and Incoherent Light Sources

obtained for the Pr3 , Yb3+ codoped system, a so-called


Energy
25 sensitized photon avalanche, in YLiF4 (YLF) [11.156–
Emitting 158] and BaY2 F8 (BYF) [11.121]. The principle scheme
20 level of the Pr-Yb system is shown in Fig. 11.39 [11.159–
ë pump CR 163]. The excitation around 840 nm corresponds to
15 a very weak ground-state absorption process (very
ESA probable into a phonon tail of the Yb3+ absorption), fol-
Part C 11.2

10 Reservoir lowed by energy transfer (process r in Fig. 11.39) from


level
Yb3+ to Pr3+ (2 F5/2 , 3 H4 ) → (2 F7/2 , 1 G4 ). The ESA
5 process (1 G4 → (1 I6 , 3 P1 )), followed by fast phonon de-
GSA CR excitation [(1 I6 , 3 P1 ) → 3 P0 ] feeds the 3 P0 level (i. e.,
Ground state
0 the emitting level). The cross-relaxation process s
level
(3 P0 , 2 F7/2 ) → (1 G4 , 2 F5/2 ) followed again by the trans-
Fig. 11.37 Scheme of the photon-avalanche process (GSA: fer process r re-feeds the reservoir level. In this way,
ground-state absorption, ESA: excited-state absorption, at each step, an increase of the population in the 1 G4
CR: cross-relaxation) level is obtained and consequently a strong population
will be build up in the 3 P0 level (because of the strong
reason is that there exist special requirements for an effi- 1 G → (1 I , 3 P ) ESA process). The upconverted emis-
4 6 1
cient avalanche process; its efficiency depends strongly sion excitation spectrum and the excited-state absorption
on the transfer rates between the ions, the ground- spectrum are shown in Fig. 11.40 indicating the good
and excited-state absorption cross sections, the ionic match between these two spectra. The peak excited-
concentration, the emission branching ratios and the state absorption cross section of the 1 G4 → (1 I6 , 3 P1 )
lifetimes of the energy levels involved. In principle it transition is about 1.5 × 10−19 cm2 .
is possible to describe the photon-avalanche excitation The laser input–output curves for Pr,Yb:YLF and
mechanism for Pr,Yb-doped systems with rate equation Pr,Yb:BYF under Ti:sapphire pumping are shown in
systems [11.113, 114, 117, 118, 120]. However, due to Fig. 11.41; the results are summarized in Table 11.5.
its complexity, it is not possible to predict the overall The realization of diode pumping using commercially
efficiency solely from knowledge of the spectroscopic available infrared laser diodes is under investigation in
parameters. several research groups. However, at the moment ion-
In Table 11.5 an overview of photon-avalanche doped fibers as materials for upconversion and avalanche
pumped Pr3+ laser systems is given. Room-temperature pumped lasers are more efficient, because they allow
avalanche-pumped laser oscillation in bulk crystals was waveguiding of both the pump and the laser beam.

ncalc (cm3) I (arb.units) I (arb.units)

1019
2 100
100
1018

10
1017 Slope 8

1
1016
Slope 2

1015 0.1
0 0
1000 0 3 6
P (mW) t (ms)
Fig. 11.38 Characteristics of the photon-avalanche excitation mechanisms. Left: pump-power dependence of the upcon-
verted emission intensity (experiment, open circles) and 3 P0 population (calculated, filled squares). Right: temporal
evolution of the upconverted emission intensity (solid line: experiment, squares: rate equation model). (After [11.120])
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 629

Table 11.5 Photon-avalanche pumped crystalline CW Pr3+ lasers in the visible spectral range (T : temperature, η: slope
efficiency)
Dopant ions Host λlaser (nm) Transition λpump (nm) T Output (mW) η (%) Ref.
Pr3+ LaCl3 644 3 P →3 F 677 80–210 K 240 25 [11.164]
0 2
Pr3+ / Yb3+ YLiF4 522 3 P →3 H 830 RT 143 7.5 [11.156–158]
1 5
639.5 3 P →3 F 830 276 15
0 2
720 3 P →3 F 830
0 3

Part C 11.2
Pr3+ /Yb3+ BaY2 F8 607.5 3 P →3 H 822, 841 RT 98 30 [11.121]
0 6
638.5 3 P →3 F 822, 841 60 15
0 2
720.5 3 P →3 F 822 45 16
0 3

Table 11.6 Other rare-earth-doped solid-state upconversion lasers; for details see the overview in [11.114, 116] (ETU: energy
transfer upconversion, STPA: sequential two-photon absorption, CT: cooperative transfer, PA: photon avalanche, CW: continuous
wave, p: pulsed, SP: self pulsed, QS: Q-switched, ML: mode-locked, IR-fl: infrared flashlamp, RT: room temperature). ∗ First
observation of laser oscillation based on an upconversion process [11.169]
Dopant ions Host λlaser (nm) λpump (nm) Pump T (K) Output η (%) Ref.
mechanism
Nd3+ LaF3 380 788 + 591 STPA ≤ 90 12 mW, CW 3 [11.165,
166]
Nd3+ LaF3 380 578 STPA ≤ 20 4 mW, CW 0.7 [11.165,
166]
Nd3+ LiYF4 730 603.6 PA ≤ 40 11 [11.165,
167]
Nd3+ LiYF4 413 603.6 PA ≤ 40 10 µW, CW 4.3 [11.165,
165, 167]
Ho3+ / Yb3+ KYF4 551 960 ETU 77 CW [11.168]
Ho3+ / Yb3+ BaY2 F8 551.5 IR-fl ETU 77 [11.169]∗
Tm3+ YLiF4 450.2, 453 781 + 647.9 STPA 77 - RT 0.2 mJ, p 1.3 [11.170]
(pulsed lasers)
Tm3+ YLiF4 450.2 784.5 + 648 STPA ≤ 70 9 mW, SP 2 [11.171,
172]
Tm3+ YLiF4 483 628 PA ≤ 160 30 mW 7.5 [11.171,
172]
Tm3+ YLiF4 483 647.9 PA ≤ 160 30 mW, SP 8 [11.171,
172]
Tm3+ Y3 Al5 O12 486 785 + 638 STPA ≤3 0.07 mW, SP 0.01 [11.173]
Tm3+ / Yb3+ BaY2 F8 455, 510, 649, 799 960 ETU RT [11.174]
Tm3+ / Yb3+ BaY2 F8 348 960 ETU 77 CW [11.175]
Tm3+ / Yb3+ BaY2 F8 348 960 ETU RT SP [11.175]
Tm3+ / Yb3+ BaY2 F8 649 1054 ETU RT 1 [11.176]
Tm3+ / Yb3+ YLiF4 810, 792 969 ETU RT 80 mW, CW [11.177]
Tm3+ / Yb3+ YLiF4 650 969 ETU RT 5 mW, CW 0.2 [11.177]

Table 11.7 Visible Er3+ lasers with direct pumping (p = pulsed operation)
Crystal Laser transition λlaser (µm) Pump T Output mode Ref.
3/2 → I15/2
Ba(Y, Er)2 F8 4S 4 0.5540 Xe lamp 77 p [11.178]
2H
9/2 → 4I
13/2 0.5617 Xe lamp 77 p [11.169, 178]
9/2 → I15/2
4F 4 0.6709 Xe lamp 77 p [11.178]
9/2 → I11/2
2H 4 0.7037 Xe lamp 77 p [11.178]
Ba(Y, Yb)2 F8 4F
9/2 →4I
15/2 0.6700 Xe lamp 77 p [11.169]
9/2 → I15/2
BaYb2 F8 4F 4 0.6700 Xe lamp 110 p [11.169, 179]
3/2 → I11/2
LiYF4 4S 4 0.551 Dye laser 300 p [11.180]
630 Part C Coherent and Incoherent Light Sources

The energy-level schemes of Erbium-doped crystals


E (103 cm–1) such as LiYF4 and LiLuF4 [11.127, 128] offer the fea-
25 sibility of realizing an upconversion laser emitting in
3
P2 1 the green spectral region (4 S3/2 → 4 I15/2 transition). As
3 I 6 + 3P 1
P0 shown in Fig. 11.42 the upconversion excitation of the
1
upper laser level 4 S3/2 requires sequential two-photon
D2 absorption (STPA) either at 810 nm or 970 nm. With
Red emission
Part C 11.2

s ESA Green emission a pump wavelength of 810 nm, the ground-state absorp-
Blue emission tion (GSA) 4 I15/2 → 4 I9/2 is followed by nonradiative
2
F5/2
1
G4 decay to the 4 I11/2 level. From there, population is taken
3
3 F4 to the 4 F5/2 level by excited-state absorption (ESA).
F3
3
3
H6 F2 Finally, the 4 S3/2 level is populated by nonradiative
3 r r s GSA decay. With a pump wavelength around 970 nm, the up-
H5
0 3H 4 2
F7/2 conversion excitation scheme of the upper laser level
3+ 3+ is very similar, however, it involves the GSA process
Pr Yb
15/2 → I11/2 and the ESA process I11/2 → F7/2 .
4I 4 4 4
Fig. 11.39 Scheme of the avalanche mechanism in Yb–Pr-doped Using a Ti:sapphire laser for excitation, vari-
systems ous rare-earth-doped fluoride crystals have shown
room-temperature CW upconversion lasing in the vis-
ó ESA –ó GSA –óSE (10–19 cm2) Iexcite (arb. units)
ible spectral range, e.g., Er3+ :LiYF4 [11.181] and
2 Er3+ :LiLuF4 [11.182]. Diode pumping of a green er-
bium-doped upconversion laser in Er3+ :LiLuF4 [11.183]
3
and in the mixed fluoride crystal Er3+ :LiKYF5 [11.184]
1.5 Excitation has been demonstrated. In the latter case, however,
signal
2
laser operation could only be achieved under chopped
1 excitation with a duty cycle of 20%.
Table 11.8 presents an overview Er-based upcon-
1 version lasers in different crystals and at various
0.5 ESA
signal wavelengths.
Besides YAlO3 most of the interesting candidates
0 0 are fluorides, due to their relatively small phonon ener-
800 820 840 860 880
–1
E (cm ) gies and correlated long lifetimes of intermediate states.
Rare-earth-doped LiLuF4 exhibits a larger splitting of
Fig. 11.40 Upconverted emission excitation spectrum and the manifolds by the crystal field compared to LiYF4
excited-state absorption spectrum of Pr3+ , Yb3+ :BaY2 F8 . and LiGdF4 , which tends to produce more-favorable
(After [11.120]) thermal occupation factors of both the upper and lower
laser levels [11.185, 186]. A reasonable overlap be-
Therefore high pump intensities over a long distance tween GSA and ESA enables two-step excitation to the
are possible, increasing the overall efficiency of the 4S 3+ using just a single pump wave-
3/2 level of Er
avalanche pumping mechanism, see the section on visi- length. The emission cross section σem at 552 nm (π
ble fiber lasers in Sect. 11.2.2. polarization) is σem = 3.5 × 10−21 cm2 . This value as
well as the GSA cross sections around 970 nm are
Er3+ lasers. The problem for the realization of directly slightly larger than the corresponding cross sections in
pumped visible Er3+ lasers is the lack of efficient pump Er3+ (1%):LiYF
 4 4 . The lifetime
 τ of the upper laser level
3/2 τ( S3/2 ) = 400 µs is slightly longer in LiLuF4
sources that have a good spectral match to the ab- 4S

sorption lines of the Er3+ ion. Therefore most visible than in LiYF4 .
Er3+ laser schemes have been realized by upconversion A multipass pumping setup has been used in order
pumping in the near-infrared spectral range, as shown to increase the absorbed pump power (Fig. 11.43). Both
in Fig. 11.42. Table 11.7 summarizes a few results of di- end faces of the 1.6 mm-long Er3+ (1%):LiLuF4 crys-
rect pumping of Er3+ obtained with Xe lamps and a dye tal have been prepared with directly coated dielectric
laser. mirrors [11.183]. One of these mirrors is highly trans-
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 631

Output power (mW) Absorbed pump power (W) Pout (mW)


0 0.5 1 1.5 2
300 100
Pr (3 %), Yb (6 %): YLiF4 ë = 638.7 nm, T = 0.8 %
Pthr = 56 mW, ç = 15 %
250 ëlaser = 639.5 nm 80 ë = 607.5 nm, T = 6 %
ëlaser = 522 nm Pthr = 85 mW, ç = 31 %
200
ë = 720 nm, T = 2 %
60

Part C 11.2
Pthr = 161 mW, ç = 16 %
150
40
100

20
50

0 0
0 1 2 3 4 5 6 0 100 200 300 400 500
Incident pump power (W) Pabs (mW)

Fig. 11.41 Input–output curves of Pr,Yb:YLF [11.157, 158] (left) and Pr,Yb:BYF (right) under avalanche pumping with
a Ti:sapphire laser

mitting for the pump wavelength and highly reflecting is focused through the mirror hole into the crystal. With
for the laser wavelength, while the other mirror is highly respect to single-pass pumping significant improvement
transmitting for the laser wavelength and highly reflect- of the performance of the Er3+ :LiLuF4 upconversion
ing for the pump wavelength (Fig. 11.43, coatings L laser could be achieved under Ti:sapphire laser excita-
and P, respectively). An additional concave mirror with tion by using this setup. The maximum CW output power
a hole drilled slightly off axis is used to realize up to was 213 mW at an incident pump power of 2.6 W. The
four passes of the pump radiation through the active slope efficiencies with respect to incident and absorbed
volume of the laser crystal. The collimated pump beam pump power were 12% and 35%, respectively. When
replacing the Ti:sapphire laser by a 3 W diode, it was
possible to realize laser-diode-pumped CW operation of
Energy (103 cm–1) this erbium-doped upconversion laser at room temper-
4
F5/2 ature for the first time [11.183]. The maximum output
4
F7/2 power was 8 mW at an incident pump power of 2.5 W.
20 2
H11/2 The absorbed power under four-pass pumping was small
4
S3/2 and estimated to be between 10% and 12%. The slope
810 nm 970 nm efficiency with respect to the absorbed pump power was
4
15 F9/2 14%. Pumped with an optically pumped semiconductor
laser operating at 970 nm, continuous-wave laser oscil-
4
I9/2 lation at 550 nm with Er3+ :LiLuF4 has been achieved
4
I11/2 with an output power of 500 mW and a slope efficiency
10
of about 30% [11.127, 128, 182, 183].
552 nm
4
I13/2 Other 4f–4f divalent and trivalent rare-earth ion
5 lasers. Besides visible lasers based on 4f–4f transitions
810 nm 970 nm of Pr3+ and Er3+ several other lasers with 4f–4f tran-
sitions in the visible spectral region have been realized
4
I15/2 as shown in Table 11.6. When compared to Pr3+ and
0
Er3+ lasers, the laser performance of all listed systems
Fig. 11.42 Energy-level scheme of Er3+ :LiLuF4 [11.127, in Table 11.6 is worse. However, at least the upconver-
128] with two possible upconversion excitation routes of sion pumped Tm3+ and Ho3+ lasers seem to have some
sequential two-photon absorption (STPA) at 810 nm or potential for improvement of laser performance in the
970 nm [11.182, 183] and emission at 552 nm visible spectral region.
632 Part C Coherent and Incoherent Light Sources

Table 11.8 Visible Er3+ lasers (ETU: energy transfer upconversion, STPA: sequential two-photon absorption, CT: cooperative
transfer, PA: photon avalanche, CW: continuous wave, p: pulsed, SP: self-pulsed, QS: Q-switched, ML: mode-locked, IR-fl:
infrared flashlamp, OPS: optically pumped semiconductor, RT: room temperature)
Host λlaser (nm) λpump (nm) Pump T (K) Output η (%) Ref.
mechanism
BaY2 F8 670 IR-fl ETU 77 [11.169]
Part C 11.2

YAlO3 550 792 + 840 STPA ≤ 77 0.8 mW, CW 0.2 [11.187]


YAlO3 550 785 + 840 STPA 34 8 mW, CW 1.8 [11.188, 189]
YAlO3 550 807 ETU 7 –63 166 mW, CW 13 [11.188]
YAlO3 550 791.3 STPA 7 –34 33 mW, CW 3.3 [11.188, 190]
+ looping
Y3 Al5 O12 561 647 + 810 STPA RT [11.191]
CaF2 855 1510 CT 77 64 mW, CW 18 [11.192]
LiYF4 551 797 or 791 (diode) STPA ≤ 90 0.2 [11.193–196]
LiYF4 551 791 (diode) ETU / STPA ≤ 90 0.1 mW, SP 0.03 [11.195]
LiYF4 551 802 (diode) ETU / STPA ≤ 77 2.3 mW, SP [11.197]
LiYF4 551 797 (diode) CT 48 100 mW, SP 5.5 [11.198]
LiYF4 702 1500 CT 10 360 µW, CW 0.06 [11.199]
LiYF4 551 810 STPA RT 40 mW, CW 1.4 [11.181]
LiYF4 551 974 STPA RT 45 mW, CW 2 [11.200, 201]
LiYF4 551 1500 ETU 80 10 mW, SP 2.9 [11.202]
LiYF4 561 1500 ETU 80 12 mW, SP 3.4 [11.202]
LiYF4 468 1500 ETU 80 0.7 mW, SP 0.2 [11.202]
LiYF4 561, 551, 544 797 ETU 49 467 mW, CW 11 [11.203]
LiYF4 551, 544 1550 CT 9 –95 34 mW, CW 8.5 [11.204, 205]
LiYF4 551, 544 1500 CT ≤ 95 0.6 µJ (50 ns), QS 2 mW, ML [11.206]
LiYF4 551 647 + 810 STPA RT 0.95 mJ, p 8.5 [11.191]
LiYF4 467 1550 CT 70 [11.116]
LiYF4 469.7 969.3 ETU ≤ 35 2 mW, CW 0.3 [11.207]
LiYF4 469.7 653.2 ETU ≤ 35 6 mW, CW 4.8 [11.207]
LiYF4 560.6 969.3 ETU ≤ 35 2 [11.207]
LiYF4 551 802 ETU ≤ 90 5 mW, SP 2 [11.165]
LiYF4 1230, 850 1530 ETU 110 [11.208]
LiLuF4 552 970 STPA RT 213 mW 35 [11.183]
968 (diode) 8 mW 14
LiLuF4 552 970 (OPS) STPA RT 500 mW (CW) 30 [11.209]
800 mW (DC: 50)
KYF4 562 647 + 810 STPA RT 0.95 mJ, p 0.5 [11.191]
LiKYF5 550 488 (Ar+ ) STPA RT 40 mW 18 [11.184]
651 (diode) 50 mW (DC: 20) 6
808 (diode) 150 mW (DC: 20) 12
BaYb2 F8 670 1540 + 1054 or 1054 ETU RT [11.210]
BaY2 F8 470, 554, 555 792.4 CT 10 [11.211]
BaY2 F8 552 792.4 CT 40 [11.211]
BaY2 F8 617, 669 792.4 CT 20 [11.211]
BaY2 F8 552, 470 ≈ 790 or ≈ 970 STPA 10 CW [11.212]
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 633

Blue upconversion laser emission in Tm-doped crys-


Crystal
tals can be achieved with STPA pumping. The energy
levels and upconversion pump mechanisms in Tm3+ are
illustrated in Fig. 11.44.
Figure 11.44a shows a pure STPA-pumped up- Ti:sapphire or
laser diode
conversion laser scheme, whereas in Fig. 11.44b, L P
Optical
upconversion pumping also requires an additional diode Lens Pump Output

Part C 11.2
cross-relaxation step between two Tm3+ ions. This mirror coupler
T = 4%
cross-relaxation process populates the intermediate 3 F4
state which is the starting level for the second step of the L: HR @ 552 nm, AR @ 970 nm
P: HR @ 970 nm, AR @ 552 nm
STPA process.
In sensitized upconversion lasers a donor ion D (the Fig. 11.43 Experimental setup for fourfold-pass pumping [11.183]
sensitizer) absorbs the pump light and transfers its exci- (HR: high reflection, AR: antireflection)
tation energy to an acceptor ion A. In many cases Yb3+
has been used as the donor D for trivalent rare-earth-ion tals, fluoride materials are preferred because of their
activators A. Through an upconversion energy transfer low phonon energies and generally larger bandgaps.
(ETU), two donor ions transfer their excitation energy The fiber material of choice is the fluorocirconate glass
successively to an acceptor. Finally the excitation en- ZBLAN (ZrF4 − BaF2 − LaF3 − AlF3 − NaF). Another
ergy of the donor is higher than the energy of an excited advantage of fibers compared to bulk crystals is that
Yb3+ ion. the transitions in glass are broadened and therefore the
Figure 11.45 shows a system with D = Yb3+ and possibility for resonant transitions or energy transfer is
A = Tm3+ . In this case a three-step STPA process is enhanced. An overview of visible fluoride fibers is given
also possible, yielding a variety of laser transitions in in [11.214].
the visible region. Nearly all rare-earth-ion-doped fluoride fiber lasers
Figure 11.46 illustrates the STPA and ETU upcon- can be pumped in the 0.63–1.2 µm region and
version mechanisms in Ho3+ and in the donor–acceptor thus take advantage of the mature semiconductor
system Yb3+ –Ho3+ . Laser emission can be gener- technology, e.g., AlGaInP (0.63–0.69 µm), GaAlAs
ated near 750 nm and 550 nm, originating from the (0.78–0.88 µm) and InGaAs (0.90–1.2 µm) and of
metastable 5 S2 , 3 F4 states. the highly developed solid-state laser technology, e.g.,
It can be seen in Table 11.6 that, besides STPA and
ETU pumping, photon avalanche (PA) pumping has also
a) Energy (103 cm–1) b) Energy (103 cm–1)
been used in a few cases (Nd3+ and Tm3+ ). 30 30
In Table 11.9 other rare-earth-ion lasers in the visible 1
D4 1
D2
spectral range based on 4f–4f transitions are listed. The
data are taken from [11.213]. 25 649 nm 25
1
G4 1
G4
Visible fiber lasers 20 20
A different and very promising approach to realize ef-
450 nm
ficient upconversion room-temperature laser oscillation 638 nm 486 nm
is the use of rare-earth-ion-doped fibers. The geome- 15 15
3 3
try of the fiber provides waveguiding of both the pump H4 H4
radiation and the stimulated emission, thus long inter- 10 10
action lengths can be realized, yielding high intensities 781 nm
3
over a long distance, a critical requirement for upcon- F4 3
F4
version lasers. This is one advantage of the fiber concept 5 5
785 nm
(for a detailed description of the fiber concept, see
the description of Yb fiber lasers in Sect. 11.2.2) com- 3 3
0 H6 0 H6
pared to bulk materials. Another requirement for visible
upconversion lasers is the existence of metastable inter- Fig. 11.44a,b Upconversion pump mechanisms for Tm3+ . (a) Se-
mediate levels to act as initial levels for an excited-state quential two-photon absorption, (b) sequential two-photon absorp-
absorption or an energy transfer process. Like in crys- tion with additional cross-relaxation (dashed line)
634 Part C Coherent and Incoherent Light Sources

Table 11.9 Visible and UV lasers based on divalent and trivalent rare-earth ions
Dopant ions Host Transition λlaser (nm) T (K) Ref.
Sm3+ 5/2 → H7/2
TbF3 4G 6 593.2 116 [11.215]
Sm2+ SrF2 5 D →7 F 696.9 4.2 [11.216]
0 1
Eu3+ Y2 O3 5 D →7 F 611.3 220 [11.217]
0 2
Eu3+ YVO4 5 D →7 F 619.3 90 [11.218]
0 2
Gd3+ 7/2 → S7/2
6P 8
Part C 11.2

Y3 Al5 O12 314.5 300 [11.219]


Tb3+ LiYF4 5 D →7 F 544.5 300 [11.220]
4 5
Ho3+ CaF2 5 S →5 I 551.2 77 [11.221]
2 8
Tm2+ 5/2 → F7/2 < 27
CaF2 2F 2 1116 [11.97, 98]
Ag+ KI, RbBr, CsBr 335 5 [11.222]

Nd3+ and Yb3+ lasers in the near-infrared spectral levels, which are thermally coupled. In Pr3+ :ZBLAN,
region. the lifetime of these coupled multiplets is in the range
40–50 µs [11.224,225]. Recently, Richter et al. obtained
Visible Pr3+ fiber lasers. As in crystals, the
praseodymium ion is very attractive for visible fiber
lasers because of its energy-level scheme (see Fig. 11.33) a) Energy (103 cm–1)
25 5
and the possibility of upconversion pumping by two- G5
step absorption, photon avalanche or energy transfer
5
processes. Laser oscillation at room temperature has 20 F3
5
been achieved in the red, orange, green and blue spec- S 2, 5F 4
647 nm
tral ranges. Some of these transitions have even been 5
15 F5
operated simultaneously [11.223]. Laser oscillation at
550 nm
room temperature originates from the 3 P0 , 3 P1 and 1 I6 753 nm
10 647 nm
5
3 I6
P2
3
3
P0 P1 5 5
I7
1
I6
647 nm
457 – 458 nm 5
0 I8
1
D2
b) Energy (103 cm–1)
512 nm
20
456 nm 5
S 2, 5F 4
1
G4
799 nm 5
15 F5
649 nm
3 5
3 F2 I4
F4
3 5
F4 2 I5
1480 nm
10 F5/2
2
F5/2 5
I6
3
H5
3
H4 960 nm 5 960 nm
5
I7
482 nm
552 nm
3 2
H6 F7/2
3+ 3+
Tm Yb 0 2
F7/2 5
I6
3+ 3+
Yb Ho
Fig. 11.45 Sensitized upconversion in Yb3+ ,Tm3+ -doped
BaY2 F8 after Trash and Johnson [11.174] with two and Fig. 11.46a,b STPA (a) and ETU (b) pumping of Ho3+
three steps in the STPA process upconversion lasers
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 635

Table 11.10 Visible Pr3+ -doped ZBLAN fiber lasers (ESA: excited-state absorption (i. e., sequential two-step absorption), ETU:
energy transfer upconversion, PA: photon avalanche, RT: room temperature)
Dopant ions λlaser (nm) Transition λpump (nm) Pump T (K) Output η (%) Ref.
mechanism
Pr3+ 635 3P
0 →3 F2 1010 + 835 ESA RT 180 mW 10 [11.227]
605 3P
0 →3 H6 1010 + 835 ESA RT 30 mW 3.3
3P →3 H5

Part C 11.2
520 1 1010 + 835 ESA RT 1 mW
491 3P
0 →3 H4 1010 + 835 ESA RT 1 mW
Pr3+ 635 3P
0 →3 F2 1020 + 840 ESA RT 54 mW 14 [11.228]
520 3P
1 →3 H5 1020 + 840 ESA RT 20 mW 5
491 3P
0 →3 H4 1020 + 840 ESA RT 7 mW 1.5
Pr3+ , Yb3+ 635 3P
0 →3 F2 849 ETU RT 20 mW [11.229]
Pr3+ , Yb3+ 635 3P
0 →3 F2 1016 diode ETU RT 6.2 mW 3.2 [11.230]
+ 833 diode
532 3 P →3 H ETU RT 0.7 mW 0.3
1 5
Pr3+ , Yb3+ 635 3 P →3 F 860 diode ETU RT 4 mW 2.2 [11.231]
0 2
602 3 P →3 H 860 diode ETU 0.2 mW
0 6
Pr3+ , Yb3+ 520 + 490 3 P →3 H 856 diode RT 1.4 mW [11.223]
1 5
+3 P0 →3 H4
Pr3+ , Yb3+ 492 3 P →3 H 1017 diode RT 1.2 mW 8.5 [11.232]
0 4
+ 835 diode
Pr3+ , Yb3+ 635–637 3 P →3 F 780–880 PA RT 300 mW 16.8 [11.161]
0 2
605–622 3 P →3 H 780–880 PA RT 45 mW 4.6
0 6
517–540 3 P →3 H 780–880 PA RT 20 mW 5
1 5
491–493 3 P →3 H 780–880 PA RT 4 mW 1.2
0 4
Pr3+ , Yb3+ 635 3 P →3 F 850 PA RT 1020 mW 19 [11.162]
0 2
Pr3+ , Yb3+ 635 3 P →3 F 850 diode PA RT 440 mW 17 [11.233]
0 2
520 3 P →3 H 850 diode PA RT 100 mW ≈4
1 5
Pr3+ , Yb3+ 635 3 P →3 F 850 diode PA RT 2W 45 [11.234, 235]
0 2
520 3 P →3 H 850 diode PA RT 0.3 W 17
1 5
Pr3+ , Yb3+ 491 3 P →3 H 850 PA RT 165 mW 12.1 [11.236]
0 4
491 + 520 3 P →3 H 850 PA RT 230 mW 14.3
0 4
+3 P1 →3 H5
491 3 P →3 H 840 diode PA RT 8 mW ≈6
0 4
Pr3+ , Yb3+ 635 3 P →3 F 838 diode PA RT ML: 550 ps [11.237]
0 2
(239 MHz)
Pr3+ , Yb3+ 603 (tunable) 3P
0 →3 H6 840, Ti:Sapphire PA RT 55 mW 19 [11.238]
634 3P
0 →3 F2 100 mW
Pr3+ 635 3P
0 →3 F2 480, diode Direct RT 94 mW 41.5 [11.226]

laser oscillation of a Pr3+ -doped ZBLAN fiber under di- green and blue wavelength regions are about one order
rect pumping with a blue semiconductor laser [11.226]. of magnitude smaller.
Output powers of 94 mW and a slope efficiency of 41.5% Generally, a double-clad fiber can be used to couple
at 635 nm were obtained. highly divergent pump radiation of near-infrared high-
In Table 11.10 the results to date with Pr3+ -doped power laser diodes into the large-numerical-aperture
ZBLAN fibers are summarized. The best results ob- inner cladding and propagate it along the fiber axis.
tained thus far, at the most efficient wavelength of On its way down the fiber, the pump radiation is gradu-
635 nm, are output powers up to 2 W and slope effi- ally absorbed in the embedded small-numerical-aperture
ciencies up to 45% [11.234]. The efficiencies in the active core. Since the number of transverse radiation
636 Part C Coherent and Incoherent Light Sources

be best provided by diffraction-limited pump radia-


tion focused onto the fiber end face and guided in the
rare-earth-ion-doped active core.
2
Ti3+: Al2O3 lasers For example, Fig. 11.47 shows a demonstration of
(1, 2) high-power upconversion laser operation under pump-
M2 ing with two dichroic coupled Ti3+ :Al2 O3 lasers
C2 tuned to pumping wavelengths near 850 nm [11.162].
Part C 11.2

1 The maximum upconversion-laser output power


Fiber was 1020 mW at an incident near-infrared total pump
M1 C1
power of 5.51 W (Fig. 11.48). The overall slope ef-
Fig. 11.47 Experimental setup of the Pr3+ ,Yb3+ -doped up- ficiency with respect to the incident pump power
conversion ZBLAN fiber laser [11.162]. M1 denotes the was 19% [11.162].
dichroic mirror, C1 an aspheric lens, M2 the dielectric Also, near-infrared high-power diode-laser bars
resonator mirror, and C2 a collimator with beam-shaping optics have been used to pump
a Pr3+ ,Yb3+ -doped ZBLAN fiber with the common
modes supported in a cylindrical fiber core depends only single-clad structure and a large-area multimode active
on the wavelength of the radiation, the core diameter, core. In this case, 4.5 W of pump power were launched
and its numerical aperture, the geometry and mater- into the fiber core, generating red output powers in ex-
ial of the active fiber core can be chosen to support cess of 2 W at 635 nm [11.234]. In the blue spectral
just one or a few transverse modes of the radiation range, a Pr3+ ,Yb3+ -doped ZBLAN-based upconver-
generated in the active core by near-infrared pumping. sion fiber laser has been demonstrated at an emission
Thus, an upconversion double-clad fiber with a suit- wavelength of 491 nm (3 P0 → 3 H4 transition of Pr3+ ).
ably chosen rare-earth-ion-doped active core can be The pump source was a single-mode diode laser emit-
used to convert the highly multimode radiation of high- ting at a wavelength of 840 nm. The maximum blue
power near-infrared laser-diode arrays into single-mode output power was 8 mW at an incident pump power
or few-mode visible laser emission with excellent beam of 200 mW [11.236].
quality. The best results in terms of upconversion laser
output power, however, have been achieved when the Other visible fiber lasers. Laser oscillation in the visible
pump radiation of a high-beam-quality laser source was spectral range has also been obtained with other rare-
launched directly into the active core of the described earth ions in ZBLAN. In Table 11.11 an overview of
fiber. This is due to the high pump intensities required these laser systems is given. A detailed description of
locally for photon-avalanche upconversion, which can these systems and their prospects is given in [11.214].

11.2.3 Near-Infrared Rare Earth Lasers


Laser output power Pout (W)

1 Ti:sapphire 1 @ ë = 850 nm Nd lasers


Ti:sapphire 1 @ ë = 852 nm
most intensively investigated class of solid-state lasers
plus Ti:sapphire 2 @ ë = 826 nm is based on Nd3+ -ion-doped materials. The Nd3+ -ion
0.8
offers various groups of laser lines in the near-IR spectral
region.
0.6

Energy-level scheme. Figure 11.49 shows transitions


0.4 from the 4 F3/2 upper laser level into the 4 I13/2 , 4 I11/2 ,
Pout, max = 1020 mW and 4 I9/2 manifolds. The specific absorption and emis-
0.2 Pthr = 202 mW sion wavelengths depend on the crystal field, which
çinc = 19 % influences the splitting within a manifold and between
0 different manifolds. As shown in Fig. 11.49 the splitting
0 0.5 1 1.5 2 2.5 3 3.5 4 4.5 5 5.5
Incident pump power Pin (W)
between the 4 I (and also between 4 F) manifolds is dom-
inated by L S coupling of the 4f electrons and is only
Fig. 11.48 Input–output characteristics of the Pr3+ ,Yb3+ -doped up- affected to second order by covalency effects caused by
conversion ZBLAN fiber laser [11.162] the crystal field. The energetic splitting between the 4 F
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 637

Table 11.11 Overview of room temperature rare earth ion doped upconversion fiber lasers. (in): incident, (l) launched,
(abs) absorbed
Active ion λlaser (nm) Transition λpump (nm) Pout (mW) η (%) Ref.
3/2 → I11/2
Nd 381 4D 4 590 0.076 0.25 (l) [11.239]
Nd 412 2P
3/2 →4I
11/2 590 0.470 1.7 (l) [11.240]
Tm 455 1 D →3 F 645 + 1064 3 1.5 [11.241]
2 4
1 G →3 H

Part C 11.2
Tm 480 4 4 1130 33 34.6 (abs) [11.242]
1123 230 25 (in) [11.243]
680 + ≈ 1100 14.8 18.9 (abs) [11.244–249]
Tm / Yb 480 1G
4 →3 H4 1070 375 [11.250]
1065 106 6.6 (in) [11.251]
1120, 1140 116 15 [11.252]
Dy 478 4F
9/2 → H15/2
6 457 (Ar+ ) 2.3 0.9 [11.253]
9/2 → H13/2
575 4F 6 10 1.5
3/2 → I15/2
Er 540 4S 4 801 23 16 [11.254, 255]
3/2 → I15/2
Er 540 4S 4 970 50 51 [11.256–258]
Ho 544 / 549 5 F →5 I / 5 S →5 I8 ≈ 640 40 22.4 (l) [11.259–263]
4 8 2
Ho 753 647 0.54 3.3 [11.259]
Tm 810 1064 1200 37 [11.264]

and 4 I levels is dominated by Coulomb interaction of the Because of the good spectral match, the total pump effi-
4f electrons, which is also only effected to second or- ciency of diode pumping is much higher than for lamp
der by covalency effects of the crystal field. Therefore, pumping. In addition the transfer efficiency of pump
the transition wavelengths of Nd-doped crystals vary in light into the crystal is much better in the case of diode
a certain range near the values given for Nd:Y3 Al5 O12 pumping, so that a total efficiency of 10% to 30% for
(Nd:YAG) in Fig. 11.49. The strongest and most com- the conversion of electrical power into laser power is
monly used laser transition 4 F3/2 → 4 I11/2 emits near achievable.
1060 nm (Fig. 11.49).
Figures 11.50 and 11.51 show as an example the ab-
sorption and emission spectra of Nd:YAG, measured at Energy (103 cm–1)
300 K. The strongest absorption is located near 808 nm
15 4
F9/2
and the strongest laser transition at 1064 nm. 4
F7/2
4
F5/2
Longitudinal and transversal diode pumping. Nd 4
F3/2
lasers are usually pumped by lamps or diode lasers.
Splitting between 4F
The first generation of Nd-doped solid-state lasers were 10 1444 nm and 4I levels by
pumped with CW krypton or pulsed xenon lamps. 1320 nm Coulomb interaction
808 nm 1064 nm
These lamps have high electrical-to-optical efficiencies 946 nm
of about 70% and are available at reasonable costs. Un- 938.5 nm
fortunately, the overlap of their emission spectra with 4
I 15/2
the narrow 4f–4f absorption spectra of Nd-doped solid- 5 Splitting of 4I (4F)
4
state laser materials is usually poor; thus the electrical to I 13/2 multipletts by
LS coupling
optical pump efficiency is low – typically a few percent.
4
In modern Nd lasers, diode lasers at 808 nm are em- I11/2
ployed as pump sources. Laser diodes typically have Stark splitting by
4
I 9/2 symmetry and strength
efficiencies of about 50% and offer several advantages 0 of crystal field
over lamp pumping. Diodes emit spectrally narrow-band
radiation (≈ 1–5 nm). Therefore, a much better overlap Fig. 11.49 Level scheme, pump and laser transitions of Nd3+ in
with the 4f–4f absorption spectra of Nd can be achieved. YAG
638 Part C Coherent and Incoherent Light Sources

area and their relatively large refractive index, laser


áabs (cm–1) óabs (10–20 cm2)
diode beams have a large divergence. Their beams also
14 10 possess large beam-quality differences in the transversal
and sagittal directions since the active area dimensions
12 Nd (1 %): YAG are usually ≈ 1 µm × 100 µm and confinement is given
çion = 1.39 × 1020 cm–3 8 only in one dimension. For power scaling, bars or ar-
10 rays of diodes must be used. This can lead to output
Part C 11.2

6
powers of up to several tens of watts. Unfortunately,
8 combination of many single diode stripes also broad-
ens the emission spectrum, while the beam quality of
6
4 the combined radiation is further decreased. So, sophis-
4
ticated pump optics such as beam shaping must often be
employed [11.265].
2
2 Several pump geometries can be used with diode
laser excitation. The common geometry to pump lasers,
0 0 which are capable of generating several watts of out-
780 800 820 840 860 880 900
Wavelength ë (nm) put power with excellent beam quality, is end pumping
(Fig. 11.52). In this geometry, pump radiation is fo-
Fig. 11.50 Absorption spectrum of Nd(1%):YAG and absorption cused into the laser crystal along the laser resonator
cross sections axis. A very good overlap of pump and laser modes can
be provided. Gain media of small volume and with short
The selective spectral pumping with diodes also absorption lengths can be used, and high population in-
leads to reduced heat deposition in the laser crystal with versions at low pump power levels can be achieved.
reduced thermal lensing effects, giving rise to improved Because most of the pump power is deposited within the
beam quality. Diffraction-limited beams can be realized volume of the TEM00 laser mode, higher-order modes
easier. usually cannot oscillate. Excellent beam quality is there-
However, there are also disadvantages of diode fore inherent. However, scaling of end-pumped lasers to
lasers. Because of their small active laser cross-sectional output powers above 20 W is difficult to achieve due to

óem (10–20 cm2)


30

Nd: YAG
25
4 4 4 4 4 4
F 3/2 I 9/2 F 3/2 I11/2 F3/2 I13/2

20

15

10

0
860 880 900 920 940 1050 1060 1070 1080 1350 1400 1450
Wavelength ë (nm)

Fig. 11.51 Emission cross section spectra of Nd:YAG


Lasers and Coherent Light Sources 11.2 Solid-State Lasers 639

possible thermally induced fracture of the laser crystal


Pump Laser resonator
within the small volume of pump absorption. diode laser
An alternative diode pumping method is side pump-
ing (Fig. 11.53, [11.266]). In this approach, the pumping
geometry is principally similar to the arrangement for
lamp pumping. One or several linear pump diode bars
are positioned around the side surface of the laser crystal.

Part C 11.2
Pump radiation is then usually imaged into the crystal
perpendicular to the laser resonator axis. The crystal is
relatively homogeneously pumped throughout its total Optics
volume, and a smaller excitation density is usually real-
ized than in diode laser end pumped systems. Because of Fig. 11.52 Diode end-pumping scheme
the use of larger gain media, however, more energy can
be deposited into the laser crystal and therefore higher ics, which have been developed with very good optical
output powers can be achieved. Since a larger laser mode quality and low scattering losses. So, the efficiency of
is present inside the crystal, higher-order modes also ceramic lasers can be as high as for crystals.
usually oscillate in these lasers. Therefore beam quality If not specified otherwise, the references for the laser
is often rather low. materials can be found in [11.213].
Nd-doped fiber lasers can also be operated in specific
configurations, see for example [11.267–278], and are Yb lasers
used in many applications. For high-power laser gener- Coherent oscillation of Yb3+ was first observed in YAG
ation, double-clad fibers are usually used. Basic aspects at 77 K [11.279]. In 1991 the first realization of a diode-
are described below in this chapter (page 650/651). pumped Yb:YAG laser [11.280] at room temperature
initialized an intensive renaissance of research on Yb-
The most important Nd lasers. The most important doped laser materials for laser diode pumping at 300 K.
Nd-doped laser materials feature relatively high emis- Yb3+ -doped solid-state lasers feature several important
sion cross sections, a relatively long upper-state lifetime advantages compared with other rare-earth lasers:
of Nd3+ , a high damage threshold, high mechanical 1. Yb3+ ions have only two states, the ground state
and chemical stability, good thermal conductivity and 2F 2
7/2 and the excited state F5/2 , which are separated
very good optical quality, see Table 11.12. Many host by an energy of about 10 000 cm−1 . Thus, there is
crystals have been investigated, including yttrium alu- no excited-state absorption of the pump and laser
minium garnet (YAG), yttrium aluminium perovskite radiation (Fig. 11.54).
(YAP or YALO), yttrium lithium fluoride (YLF) and 2. The quantum efficiency of Yb3+ is close to unity.
yttrium vanadate (YVO). Very efficient and compact
diode-pumped lasers with slope efficiencies of over
60% have been demonstrated in many Nd-doped laser
Fiber holder Reflector
materials.
HR 808 nm
Nd:YAG is still regarded as the most important solid-
state laser. Due to their very good optical and mechanical
properties, diode-pumped Nd:YAG lasers are robust and
reliable. They are in use in many applications. Within Laser rod
the last few years Nd:YAG have also become available Reflector d f–f
as ceramics with high optical quality. Flow tube
The vanadates Nd:YVO and Nd:GVO emit polarized
radiation and exhibit large cross sections and gain.

Nd laser wavelength and materials. A variety of Nd 16 fibers


lasers have been reported so far. Tables 11.13, 14, 15 list (CW 10W fiber-coupled
diode lasers, Æ 800 µm, NA 0.2) 32 mm
laser materials and their laser wavelengths which have
been observed at 300 K on the transitions 4 F3/2 → 4 I9/2 , Fig. 11.53 Diode side (transversal) pumping scheme
4I 4
11/2 and I13/2 . The tables also list Nd-doped ceram- [11.266]
640 Part C Coherent and Incoherent Light Sources

Table 11.12 Important host materials for Nd3+ [11.285]


Host YAG YAlO (FAP) YVO GVO YLF
Chemical formula Y3 Al5 O12 YAlO3 YVO4 GdVO4 YLiF4
Lattice symmetry Cubic Orthorhombic Tetragonal Tetragonal Tetragonal
Space group 1a3d Pnma 141 /amd 141 /amd 141 /a
Lattice constant (Å) 12.00 a = 5.33 a = 7.120 a = 7.123 a = 5.18
b = 7.37 c = 6.289 b = 6.291 c = 10.74
Part C 11.2

c = 5.18
Density of Nd sites (1% doping) 1.39 1.96 1.255 1.25 1.39
Heat conductivity (Wm−1 K−1 ) 11–13 11 ∼ 5 –12 a ∼ 8 –12 a 6
dn i / dT (10−6 K−1 ) 9.9 14.5(a) 8.5(a) −0.9(a)
9.7(b) 3.0(c) −2.9(c)
dL/ dT (10−6 K−1 ) 8.2 4.4(a) 3.1(a) 1.6(a) 13(a)
10.8(b) 7.2(c) 7.3(c) 8(c)
9.5(c)
Max. phonon energy (cm−1 ) 700 550 850 490
Refractive indices n = 1.822 n a = 1.9260 n o = 1.958 n o = 1.972 n o = 1.454
n b = 1.9118 n e = 1.2168 n e = 1.2192 n e = 1.477
n c = 1.9346
τ(4 F3/2 ) (µs) 250 160 97 100 500
λabs (nm) 808 813 (E  a) 808 808 792
σabs (10−20 cm2 ) 7.9 7.2 (E  a) 60 (π) 54 (π) 14 (π)
12 (σ) 12(σ) 1.2(σ)
λlaser (4 I11/2 ) (nm) 1064 1080 (E  a) 1064 1063 1047 (π)
1054 (σ)
σem (4 I11/2 ) (10−20 cm2 ) 29 25 (E  a) 123 (π) 125 (π) 1.5 (π)
52 (σ) 61 (σ) 1.5 (σ)
∆λ(4 I11/2 ) (nm) 0.8 2.5 (E  a) 1.0 (π) 1.2 (π) 1.5 (π)
1.5 (σ) 1.3 (σ) 1.5( σ)
λlaser (4 I9/2 ) (nm) 946 930 914 (π) 912 (π) 904 (π)
915 (σ) 912 (σ) 909 (σ)
σem (4 I9/2 ) (10−20 cm2 ) 3.9 4.1 (E  a) 4.8 (π) 6.6 (π) 1.2 (π)
4.3(σ) 5.6 (σ) 1.3 (σ)
∆λ (nm) 1.0 2.5 (E  a) 2.8 (π) 2.5 (π) 3.0(π)
3.4 (σ) 3.3 (σ) 3.0 (σ)
a The published data of heat conductivities of the vanadates YVO and GVO differ considerably [11.281–284]

3. Due to the small Stokes shift and the related small to a few milliseconds, which implies greater en-
quantum defect (typically 500 cm−1 ) heat generation ergy storage efficiency, especially for Q-switched
in the lasing process of Yb3+ is small and makes it operation with diode pumping.
a suitable ion for high-average-power lasers.
4. The small ionic radius of Yb3+ compared to that One disadvantage of Yb3+ -doped lasers is that they
of other rare-earth ions favors its incorporation into operate in a quasi-three-level scheme with temperature-
Y-based host crystals such as YAG, allowing higher dependent reabsorption at the laser wavelength. This
dopant concentration and thus shorter gain elements leads to an increased threshold compared to a four-level
such as discs. scheme, because the pump must bleach the reabsorption
5. Yb3+ ions exhibit a relatively broad emission band losses (see the section on basic spectroscopic properties
which leads to tunability and the generation of ultra- in Sect. 11.2.1).
short pulses. Figures 11.55 and 11.56 show as an example
6. The radiative lifetime of the laser level ranges in dif- the absorption and emission cross section spectra of
ferent crystals from a few hundred microseconds Yb:YAG [11.286]. When pumped near the absorption
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 641

Table 11.13 Laser wavelengths of the 4 F3/2 → 4 I9/2 transi- Table 11.14 Laser wavelengths of the 4 F3/2 → 4 I11/2 tran-
tion at 300 K [11.213] sition at 300 K [11.213]
Wavelength (nm) Material Wavelength Material
0.8910 Y3 Al5 O12 0.97 (transition RbPb2 Br5 [11.309]
5/2 , H9/2 → I11/2 )
4F 2 4
0.8999 Y3 Al3 O12
0.901 Sr1−x Lax Mgx Al12−x O19 [11.287] 1.0369 CaF2 − SrF2

Part C 11.2
0.9106 Ba3 LaNb3 O12 1.0370 CaF2
0.910 LiLuF4 [11.285] 1.0370–1.0395 SrF2
0.912 Y2 SiO5 1.04065–1.0410 LaF3
0.912 YVO4 [11.288] 1.0410 CeF3
0.912 GdVO4 [11.289–291] 1.0412 KYF4
0.914 YVO4 [11.292] 1.042– 1.075 Na0.4 Y0.6 F2.2
0.916 LuVO4 [11.293, 294] 1.0445 SrF2
0.930 YAlO3 [11.213, 295] 1.046– 1.064 LiNdP4 O12
0.9312 YAlO3 1.0461 CaF2 − YF3
0.936 Gd3 Sc2 Ga3 O12 1.0461–1.0468 CaF2
0.9385 Y3 Al5 O12 1.047 LiGdF4
≈ 0.94 Y3 Al5 O12 [11.296] 1.047 LiNdP4 O12
0.941 CaY2 Mg2 Ge3 O12 1.047 LiYF4
0.9458–0.9464 Y3 Al5 O12 [11.297] 1.047– 1.078 NdP5 O14
0.946 Y3 Al5 O12 [11.213, 298–306] 1.0471 LiYF4
0.946 Y3 Al5 O12 ceramic [11.307] 1.0472 LiLuF4
0.9660 YAlO3 1.0475 LaBGeO5
0.966 Sc2 O3 [11.308] 1.0477 Li(Nd, La)P4 O12
1.0477 Li(Nd, Gd)P4 O12
1.048 Li(Bi, Nd)P4 O12
peaks at 940 nm or 970 nm, the Stokes shift to the lasing
1.048 Li(Nd, La)P4 O12
wavelength at 1030 nm corresponds to less than 10%,
1.048 Li(Nd, Gd)P4 O12
which allows in principle a slope efficiency of more
than 90%. 1.048 K5 (Nd, Ce)Li2 F10
1.0481 LiKYF5
Yb3+ thin-disc lasers. In connection with the power 1.0482 LaBGeO5
scaling of diode-pumped Yb lasers Giesen et al. [11.310] 1.0482 NaLa(MoO4 )2
invented the thin-disc laser concept as a pump and 1.0486 LaF3 − SrF2
resonator design for high-power lasers (Fig. 11.57). 1.049– 1.077 NaNdP4 O12
The active medium is a thin circular disc, which is 1.0491 SrAl12 O19
coated for both the pump and laser wavelengths with 1.0493 Sr2 Y5 Fl9
a highly reflecting (HR) dielectric mirror on the rear 1.0495 BaY2 F8
side and with an antireflection coating on the front side. 1.0495 GdF3 − CaF2
The disc is then bonded with the rear HR side to a heat 1.0497 SrAl2 O4
sink. The resonator is formed by the coated crystal and 1.0498 Ca2 Y5 F19
an output coupler. The pump light is provided by fiber- 1.0498 SrAl12 O19
coupled laser diodes which are focused onto the crystal. 1.05 KNdP4 O12
Since the thin crystal disc only absorbs a small fraction 1.05 NdP5 O14
of the pump light during one pass through the crystal, the 1.05 LaP5 O14
pump light is reflected back into the disc several times 1.05 LiLuF4
by a parabolic mirror and the folding prism [11.311]. Up
1.0500 CaF2 − ScF3
to a total of 32 pump light passes may be used.
1.0505 (Nd, La)P5 O14
Due to the geometrical setup a nearly one-
1.0505 5NaF − 9YF3
dimensional thermal gradient along the laser axis can
642 Part C Coherent and Incoherent Light Sources

Table 11.14 (continued) Table 11.14 (continued)


Wavelength Material Wavelength Material
1.0506 5NaF − 9YF3 1.0543 BaF2 − CeF3
1.0507 CdF2 − ScF3 1.0543 SrF2 − ScF3
1.051 NaNdP4 O12 1.05436 Ba2 MgGe2 O7
1.051 YP5 Ol4 1.05437 Ba2 ZnGe2 O7
Part C 11.2

1.051 (La, Nd)P5 O14 1.0547 LaMgAl11 O19


1.051 CeP5 O14 1.05499 CsY2 F7
1.051 GdP5 O14 1.055 Na3 Nd(PO4 )2
1.051 NdP5 O14 1.055 K3 (La, Nd)(PO4 )2
1.0511 (Nd, La)P5 O14 1.055 Na3 (La, Nd)(PO4 )2
1.0512 NdP5 O14 1.0551 Pb5 (PO4 )3 F
1.0512 (Nd, La)P5 O14 1.0552 LaMgAl11 O19
1.0512 (Y, Nd)P5 O14 1.0554 LiNdP4 O12
1.0513 NdP5 O14 1.0554 KY3 F10
1.0515 YP5 O14 1.0555 CsGd2 F7
1.0515 NdP5 O14 1.0555 Ba5 (PO4 )3 F
1.052 (Nd, La)P5 O14 1.0556 SrF2 − LuF3
1.052 KNdP4 O12 1.0560 SrF2 − LuF3
1.052 K5 NdLi2 F10 1.0566 La2 Si2 O7
1.052 Y3 Al5 O12 1.0567 SrF2 YF3
1.0521 BaF2 − YF3 1.0569 NdGaGe2 O7
1.0521 NdP5 O14 1.0570 GdGaGe2 O7
1.0521 YF3 1.0572 LaSr2 Ga11 O20
1.0525 YP5 O14 1.0573 CaMoO4
1.0526 BaF2 − GdF3 1.0575 CsLa(WO4 )2
1.0528 SrF2 − GdF3 1.0576 SrAl4 O7
1.0529 NdP5 O14 1.0576 SrMoO4
1.053 LiYF4 1.0576 La2 Si2 O7
1.053 (La, Nd)P5 O14 1.058 Gd3 Sc2 Ga3 O12
1.053–1.062 Ca3 (Nb, Ga)2 Ga3 O12 1.0582 Ca3 Ga4 O9
1.0530 LiYF4 1.0582–1.0597 CaWO4
1.0530 BaY2 F8 1.0583 Y3 Sc2 Ga3 O12
1.0530 CaF2 − LuF3 1.0584 Y3 Sc2 Ga3 O12 : Cr
1.0530–1.059 LaMgAl11 O19 1.0584 Y3 Sc2 Ga3 O12
1.0531 LiLuF4 1.0584 CaY2 Mg2 Ge3 O12
1.0532 LiKYF5 1.0585 YAlO3
1.0534–1.0563 BaF2 − LaF3 1.0585 LiLa(MoO4 )2
1.0535 Lu3 Al5 O12 1.0585 Sr5 (PO4 )3 F
1.0535–1.0547 CaF2 − SrF2 − BaF2 − YF3 − LaF3 1.0585 CaF2 − SrF2 − BaF2 − YF3 − LaF3
1.0537 BaF2 − CeF3 1.0585 KLa(MoO4 )2
1.0539–1.0549 α − NaCaYF6 1.0586 Sr5 (PO4 )3 F
1.054 Gd3 Ga5 O12 1.0586 PbMoO4
1.054 LaAl11 MgO19 1.0587 KLa(MoO4 )2
1.054–1.086 LaAl11 MgO19 1.0587 CaWO4
1.0540 CaF2 − YF3 1.0588 Ca3 (Nb, Ga)2 Ga3 O12
1.0540 BaF2 1.0589 SrF2 − CeF3 − GdF3
1.0540 CaF2 − YF3 1.0589 Y3 Ga5 O12
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 643

Table 11.14 (continued) Table 11.14 (continued)


Wavelength Material Wavelength Material
1.05896 CaMg2 Y2 Ge3 O12 1.060 LaB3 O6 [11.326]
1.059 (La, Sr)(Al, Ta)O3 1.0600 Gd3 Ga5 O12
1.059 BaLaGa3 O7 1.0601 GdGaGe2 O7
1.059 NaY(WO4 )2 1.0603 Y3 Ga5 O12

Part C 11.2
1.059 Na1+x Mgx Al11−x O17 1.0603 Gd2 (WO4 )3
1.059 Na2 Nd2 Pb6 (PO4 )6 Cl2 1.0603–1.0632 CaF2 − YF3
1.059 Sr5 (PO4 )3 F [11.312] 1.0604 HfO2 − Y2 O3
1.0590 SrF2 − CeF3 1.0604 NaLuGeO4
1.0590 Gd3 Ga5 O12 waveguide [11.313] 1.0605 SrF2 − ScF3
1.0591 Gd3 Ga5 O12 1.0606 Gd2 (MoO4 )3
1.0591 Lu3 Sc2 Al3 O12 1.0606 Gd3 Ga5 O12
1.0591 LaGaGe2 O7 1.0606 Gd3 Ga5 O12 waveguide [11.313]
1.0593 Sr4 Ca(PO4 )3 F 1.0607 Sr3 Ca2 (PO4 )3
1.0594 Lu3 Ga5 O12 1.0607 CaF2 − ScF3
1.0595 5NaF − 9YF3 1.0608 ZrO2 − Y2 O3
1.0595 Y3 Sc2 Al3 O12 1.0608 Nd3 Ga5 O12
1.0595 NaLa(MoO4 )2 1.0608 NaGaGe2 O7
1.0595 BaLaGa3 O7 1.0609 Lu3 Ga5 O12
1.0596 CaAl4 O7 1.0609 NaYGeO4
1.0596 Ca3 Ga2 Ge3 O12 1.061 Ca2 Al2 SiO7
1.0596 SrF2 1.061 BaGd2 (MoO4 )4
1.0597 Ca3 Ga2 Ge3 O12 1.061 CaMoO4
1.0597–1.0583 SrF2 − LaF3 1.061 YVO4 [11.327]
1.0597–1.0629 α − NaCaYF6 1.061 CaLa4 (SiO4 )3 O
1.0599 Lu3 Sc2 Al3 O12 1.0610 Ca2 Ga2 SiO7
1.0599 LiGd(MoO4 )2 1.0610 7La2 O3 − 9SiO2
1.05995 Gd3 Sc2 Al3 O12 1.0610–1.0627 Y3 Al5 O12
≈ 1.06 (Gd, Ca)3 (Ga, Mg, Zr)5 O12 : Cr 1.0612 Gd3 Sc2 Ga3 O12
≈ 1.06 CaGd4 (SiO4 )3 O 1.0612 CaLa4 (SiO4 )3 O
≈ 1.06 Ca4 YO(BO3 )3 [11.314] 1.0612 Ca3 (Nb, Ga)2 Ga3 O12
≈ 1.06 Y3 Al5 O12 [11.296] 1.0613 Ca4 La(PO4 )3 O
≈ 1.06 Y3 Sc1.0 Al4.0 O12 ceramic [11.315] 1.0613 Ba2 NaNb5 O15
≈ 1.06 Gd3 Sc2 Al3 O12 1.0613 Gd3 Sc2 Ga3 O12
≈ 1.06 GdAl3 (BO3 )4 [11.316] 1.0615 Ca(NbO3 )2
≈ 1.06 NaLa(MoO4 )2 1.0615 Y3 Al5 O12
≈ 1.06 NaGd(WO4 )2 1.0615 Lu3 Al5 OI
2
≈ 1.06 NdAl3 (BO3 )4 1.0615 Y3 Sc2 Ga3 O12
≈ 1.06 YAl3 (BO3 )4 [11.213, 317] 1.0615 Ba0.25 Mg2.75 Y2 Ge3 O12
≈ 1.06 Gd3 Ga5 O12 1.0615 NaGdGeO4
≈ 1.06 GdVO4 [11.213, 318–320] 1.0615 Y3 Al5 O12
≈ 1.06 YVO4 [11.319, 320] 1.0615–1.0625 Ca(NbO3 )2
≈ 1.06 La0.2 Gd0.8 VO4 [11.319, 321] 1.0618 Sr2 Ca3 (PO4 )3 F
1.060 Gd3 Ga5 O12 : Cr 1.0618 SrAl12 O19
1.060 Ca4 GdO(BO3 )3 1.0618 CaF2 − ScF3
[11.213, 322–324] 1.0618 LaNbO4
1.060 Ca4 YO(BO3 )3 [11.325] 1.062 LaSc3 (BO3 )4 [11.213, 328]
644 Part C Coherent and Incoherent Light Sources

Table 11.14 (continued) Table 11.14 (continued)


Wavelength Material Wavelength Material
1.0620 Gd3 Sc2 Al3 O12 1.064 Y3 Al5 O12 ceramic [11.315, 333–346]
1.0620 Lu3 Sc2 Al3 O12 1.064 Y3 Al5 O12 : Fe
1.0621 SrAl12 O19 1.064 Y3 Al5 O12 : Ti
1.0621 Gd3 Ga5 O12 1.064 Y3 Al5 O12 : Cr, Ce
Part C 11.2

1.0622 Y3 Sc2 Al3 O12 1.064 Y3 Al5 O12 : Ho


1.0623–1.10585 CaF2 − SrF2 − BaF2 − YF3 − LaF3 1.064 Y3 Al5 O12 : Er
1.0623 Lu3 Ga5 O12 1.064 YVO4 [11.213, 347–350]
1.0623 CaF2 − LuF3 1.064 YVO4 single crystal fiber [11.351]
1.0623–1.0628 CaF2 1.064 LaF3
1.0624 LaNbO4 1.064 KGd(WO4 )2 [11.352, 353]
1.0625 Y3 Ga5 O12 1.064 La3 Ga5.5 Ta0.5 O14 [11.354]
1.0625 YVO4 1.0640 La3 Ga5 SiO14
1.0628 SrWO4 1.0640–1.0657 CaF2 − CeF3
1.0629 Ca5 (PO4 )3 F 1.06405–1.0654 YAlO3
1.0629 α − NaCaYF6 1.0641 Y3 Al5 O12 : Cr
1.0629 Bi4 Si3 O12 1.0641 YVO4
1.0629–1.0656 CdF2 − YF3 1.0641 La3 Ga5.5 Ta0.5 O14
1.063 GdVO4 [11.329] 1.06415 Y3 Al5 O12
1.063 Gd3 Sc2 Ga3 O12 : Cr 1.06415 Y3 Al5 O12 [11.355]
1.063 SrWO4 1.0642 Ca3 Ga2 Ge3 O12
1.063 Na5 (Nd, La)(WO4 )4 1.0642 NaBi(WO4 )2
1.063 NdAl3 (BO3 )4 1.06425 Lu3 Al5 O12
1.063 (La, Nd)P5 O14 1.0643 SrMO4
1.063 NdAl3 (BO3 )4 1.0644 Bi4 Ge3 O12
1.0630 Ca5 (PO4 )3 F 1.0645 CaF2 − LaF3
1.0632 CaF2 − YF3 − NdF3 1.0645 La3 Ga5.5 Nb0.5 O14
1.0632 CaF2 − YF3 1.0645 La3 Ga5 SiO14
1.0633–1.0653 α − NaCaCeF6 1.0645 YAlO3
1.06335–1.0638 LaF3 1.0645 YAlO : Cr
1.0634 YVO4 1.0646 Y3 Al5 O12
1.0635 LaF3 − SrF2 1.0646 KLa(MoO4 )2
1.0635 NdAl3 (BO3 )4 1.0647 CeCl3
1.0635 NaLa(WO4 )2 1.0648 YVO4
1.0635 (Nd, Gd)Al3 (BO3 )4 1.0649 CaY2 Mg2 Ge3 O12
1.0635 Bi4 (Si, Ge)3 O12 1.065 GdVO4
1.0635 CaF2 − LuF3 1.065 (Nd, Gd)Al3 (BO3 )4
1.0637–1.0670 Y3 Al5 O12 1.065 Sr5 (VO4 )3 Cl
1.06375–1.0672 Lu3 Al5 O12 1.065 Sr5 (VO4 )3 F
1.0638 CeF3 1.0650 La3 Ga5 GeO14
1.0638 CaAl4 O7 1.0650 RbNd(WO4 )2
1.0638 NaBi(WO4 )2 1.0652 CaWO4
1.0638 NdP5 O14 1.0652 CdF2 − LuF3
1.0638 Ca3 Ga2 Ge3 O12 1.0653–1.0633 α − NaCaCeF6
1.0638–1.0644 (Y, Ce)3 Al5 O12 1.0653 NaLa(MoO4 )2
1.0639 Ca3 Ga2 Ge3 O12 1.0653–1.0665 NaLa(MoO4 )2
1.064 Y3 Al5 O12 [11.213, 301, 330–332] 1.0654 CaF2 − GdF3
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 645

Table 11.14 (continued) Table 11.14 (continued)


Wavelength Material Wavelength Material
1.0654 NdGaGe2 O7 1.070 La2 Be2 O5
1.0656 CdF2 − YF3 1.0701 Gd2 (MoO4 )3
1.0657–1.0640 CaF2 − CeF3 1.0701–1.0706 KLu(WO4 )2
1.0657 CaF2 1.0706 KY(WO4 )2

Part C 11.2
1.0658 LiLa(MoO4 )2 1.0706 LaSr2 Ga11 O20
1.0658 CsNd(MoO4 )2 1.0711 Y2 SiO5
1.0658 LuVO4 [11.356] 1.0714 KLu(WO4 )2
1.0659 GdGaGe2 O7 1.0714–1.0716 KLu(WO4 )2
1.066 Nd(Ga, Cr)3 (BO3 )4 1.0715 Y2 SiO5
1.066 K5 Nd(MoO4 )4 1.0716–1.0721 KLu(WO4 )2
1.066 K5 Bi(MoO4 )4 1.0720 CaSc2 O4
1.0661 CaF2 1.0721 KLu(WO4 )2
1.0664–1.0672 YVO4 1.07255–1.0730 YAlO3
≈ 1.0665 CdF2 − LaF3 1.0726 YAlO3
1.0666 CdF2 1.0729 YAlO3
1.0667 CdF2 − GeF3 1.073 KLu(WO4 )2 [11.357]
1.0667 NaGd(MoO4 )2 1.0737 Y3 Al5 O12
1.0668 CdF2 − LaF3 ≈ 1.074 Y2 O3 − ThO2 − Nd2 O3
1.0669 KY(MoO4 )2 1.074 SrAl12 O19
1.067 Ca3 (VO4 )2 1.0741 Gd2 O3
1.0670 La3 Ga5 SiO14 1.0741 Y2 SiO5
1.0672 CaY4 (SiO4 )3 O 1.0742 Y2 SiO5
1.0672 CdF2 − GdF3 1.0746 Y2 O3
1.0672 KGd(WO4 )2 1.0746 Y2 O3 ceramic [11.358]
1.0672 La3 Ga5 SiO14 1.075 La2 O2 S
1.0673 GaMoO4 1.0757 Sr3 Ga2 Ge4 O14
1.0673 La3 Ga5 SiO14 1.0759 LuAlO3
1.0674 NaY(MoO4 )2 1.0759 Lu2 O3 ceramic [11.359]
1.0675 LuAlO3 1.0760 GdAlO3
1.0675 Na2 Nd2 Pb6 (PO4 )6 Cl2 1.0775–1.0845 CaYAlO4
1.0675 Nd3 Ga5 SiO14 1.0780 Y3 Al5 O12
1.0675 Nd3 Ga5 GeO14 1.0780–1.086 LaMgAl11 O19
1.068 Na2 Nd2 Pb6 (PO4 )6 Cl2 1.0782 Y2 SiO5
1.0680 Nd3 Ga5 GeO14 1.0782–1.0815 YAlO3
1.0682 Y3 Al5 O12 1.0785 LuScO3
1.0687–1.0690 KY(WO4 )2 1.0786 CaAl4 O7
1.0688 Ga3 Ga2 SiO7 1.0786 Y2 O3 ceramic [11.360]
1.0688 Ca2 Ga2 Ge4 O14 1.0788 Ca2 Ga2 SiO7
1.0688 KY(WO4 )2 1.0789 Gd2 O3
1.0689 NdGaGe2 O7 1.079 La2 Be2 O5
1.0690 GdAlO3 1.0790 La2 Be2 O5
1.0690 Ca3 Ga2 Ge4 O14 1.0790 Lu2 SiO5
1.0694 Sr3 Ga2 Ge4 O14 1.07925 Lu2 SiO5
1.0698 La2 Be2 O5 1.0795 YAlO3
1.07 KPb2 Br5 [11.309] 1.0795–1.0802 YAlO3
1.07 RbPb2 Br5 [11.309] 1.0796 YAlO3
646 Part C Coherent and Incoherent Light Sources

Table 11.14 (continued) Table 11.15 Laser wavelengths of the 4 F3/2 → 4 I13/2 tran-
Wavelength Material
sition at 300 K [11.213]
1.08 Y2 O3 Wavelength Material
1.08 YAlO3 [11.360] 1.18 (transition RbPb2 Br5 [11.309]
5/2 , H9/2 → I13/2 )
4F 2 4
1.080 Lu2 O3 ceramic [11.359]
1.0804 LaAlO3 1.3 KNdP4 O12
Part C 11.2

1.0806 CaYAlO4 1.3 NdAl3 (BO3 )4


1.0812 Sc2 SiO5 1.302 KYF4
1.08145 Sc2 SiO5 1.304– 1.372 (La, Nd)P5 O14
1.0817 LaMgAl11 O19 1.3065 SrAl12 O19
1.0824 LaMgAl11 O19 1.307 KYF4
1.082 Sc2 O3 [11.308] 1.3070 5NaF − 9YF3
1.082–1.084 LaMgAl11 O19 1.311– 1.334 NaNdP4 O12
1.0828 SrAl4 O7 1.313 LiYF4
1.0829–1.0859 LiNbO3 1.3133 LiLuF4
1.083 YAlO3 1.3150 Ca3 Ga2 Ge3 O12
1.0832 LuAlO3 1.316– 1.340 LiNdP4 O12
1.0832–1.0855 YAlO3 1.317 Li(La, Nd)P4 O12
1.0843 YScO3 1.317 LiNdP4 O12
1.0845 YAlO3 1.3170 CeF3
1.0846 LiNbO3 1.3175 BaF2
1.085 LiNbO3 : Mg 1.318 Y3 Al5 O12
1.08515 GdScO3 1.318 BaY2 F8
1.0868 CaSc2 O4 1.3185 CaF2 − GdF3
≈ 1.0885 CaF2 − CeO2 1.3185 BaF2 − LaF3
1.0885–1.0889 CaF2 1.3185 KY3 F10
1.0909 YAlO3 1.3187 Y3 Al5 O12
1.091 Ca4 GdO(BO3 )3 [11.322] 1.3188 Y3 Al5 O12
1.0921 YAlO3 1.319 Y3 Al5 O12 [11.330, 361]
1.0922–1.0933 LiNbO3 1.319 LiNdP4 O12
1.093 LiNbO3 1.319 Y3 Ga5 O12
1.0933 LiNbO3 1.319 Y3 Al5 O12 ceramic [11.362]
≈ 1.094 LiNbO3 : MgO 1.319– 1.325 (Y, Nd)P5 O14
1.0989 YAlO3 1.3190 Ca2 Y5 F19
1.1054 Y3 Al5 O12 1.3190 CaF2 − LaF3
1.1119 Y3 Al5 O12 1.3190 CaF2 − CeF3
1.1158 Y3 Al5 O12 1.3190 Sr2 Y5 F19
1.1225 Y3 Al5 O12 1.3190 α − NaCaCeF6
≈ 1.32 Y3 Al5 O12 ceramic [11.334]
1.32 Gd3 Sc2 Ga3 O12 : Cr
be reached within the crystal. This setup minimizes the 1.32 NdP5 O14
formation of thermal lenses, and therefore yields bet- 1.32 (La, Nd)P5 O14
ter beam quality at high powers compared to a rod laser. 1.32 K(Nd, Gd)P4 O12
Multiple passes of the pump radiation through the crystal 1.32 YLiF4 [11.363]
increase the absorption efficiency and also the effective 1.320 NaNdP4 O12
pump power density in the crystal. Therefore, the thin
1.3200 SrF2 − LuF3
disc design is suitable for quasi-three-level systems such
1.3200 BaF2 − YF3
as Yb3+ . Figure 11.58 shows the input versus output
1.3200 Y3 Al5 O12
power of a thin-disc Yb:YAG laser [11.311]. CW output
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 647

Table 11.15 (continued) Table 11.15 (continued)


Wavelength Material Wavelength Material
1.3200 YP5 O14 1.3340 PbMoO4
1.3208 LiLuF4 1.3342 KLa(MoO4 )2
1.3209 Lu3 Al5 O12 1.3342 Lu3 Al5 O12
1.3209 Ba5 (PO4 )3 F 1.3342 NaBi(WO4 )2

Part C 11.2
1.3212 LiYF4 1.3345 SrAl4 O7
1.3225 CaF2 1.3347 Ca5 (PO4 )3 F
1.323 NdP5 O14 1.3347 SrWO4
1.323 (La, Nd)P5 O14 1.3350 KLa(MoO4 )2
1.324 (La, Nd)P5 O14 1.3350 Y3 Al5 O12
1.3245 CdF2 − YF3 1.3354 CaLa4 (SiO4 )3 O
1.3250 SrF2 − LaF3 1.3355 NaLa(WO4 )2
1.3250 SrF2 1.3360 Y3 Sc2 Al3 O12
1.3255 SrF2 − CeF3 1.3360 Gd3 Sc2 Al3 O12
1.3260 SrF2 − GdF3 1.3360 Lu3 Sc2 Al3 O12
1.3270 CaF2 − YF3 13360 Y3 Sc2 Al3 O12
1.3270 BaF2 1.3360 CdF2 − CeF3
1.3270 Ca3 (Nb, Ga)2 Ga3 O12 1.3365 Ca2 Ga2 SiO7
1.328 Sr5 (PO4 )3 F [11.213, 364] 1.3365 CdF2 − GaF3
1.3280 BaF2 − LaF3 1.3365 CdF2 − LaF3
1.3285 α − NaCaYF6 1.3370 CaF2 − YF3
1.3285 SrF2 − ScF3 1.3370 CaWO4
1.3298 CsLa(WO4 )2 1.3370 Gd3 Ga5 O12
1.3298 GdGaGe2 O7 1.3370 LiLa(MoO4 )2
1.330 CaF2 − LuF3 1.3375 α − NaCaYF6
1.3300 Gd3 Ga5 O12 1.338 Y3 Al5 O12 [11.365]
1.3300 CdF2 − ScF3 1.338 Y3 Ga5 O12
1.3303 NdGaGe2 O7 1.338 Sr5 (PO4 )3 F [11.366]
1.3305 HfO2 − Y2 O3 1.3380 Ca(NbO3 )2
1.3305 Y3 Ga5 O12 1.3380 NaLa(MoO4 )2
1.3310 LaF3 1.3381 Y3 Al5 O12
1.3310 Y3 Sc2 Ga3 O12 1.3382 Y3 Al5 O12
1.3310 NaLuGeO4 1.3385 NaGd(MoO4 )2
1.3315 LaF3 − SrF2 1.3387 Lu3 Al5 O12
1.3315 Lu3 Ga5 O12 1.339 YF3
1.3315 Gd3 Ga5 O12 1.3390 CaWO4
1.3315 Ca3 Ga2 Ge3 O12 ≈ 1.34 Y3 Al5 O12 [11.296, 367]
1.3317 Ca3 Ga2 Ge3 O12 ≈ 1.34 YAlO3 [11.360]
1.3320 CeF3 ≈ 1.34 GdVO4
1.3320 ZrO2 − Y2 O3 [11.213, 319, 320, 368–372]
1.3320 Ca3 Ga4 O9 ≈ 1.34 YVO4 [11.213, 319, 320]
1.3325 SrMoO4 ≈ 1.34 La0.2 Gd0.8 VO4 [11.319, 321]
1.3325 NaYGeO4 ≈ 1.34 LuVO4 [11.373]
1.3326 Lu3 Al5 O12 ≈ 1.34 GdAl3 (BO3 )4 [11.316]
1.3334 NaGdGeO4 1.3400 LiGd(MoO4 )2
1.3338 Y3 Al5 O12 1.3400 YAlO3
1.3340 CaWO4 1.3407 Bi4 Si3 O12
648 Part C Coherent and Incoherent Light Sources

Table 11.15 (continued) Table 11.15 (continued)


Wavelength Material Wavelength Material
1.341 NdAl3 (BO3 )4 1.3585 CaF2 − YF3
1.3410 Y3 Al5 O12 1.3585 Y2 SiO5
1.3410 Lu3 Al5 O12 1.3585 Lu2 SiO5
1.3410 YAlO3 1.3595 LaF3
Part C 11.2

1.3413 YAlO3 1.3600 α − NaCaYF6


1.3414 YAlO3 [11.213, 374, 375] 1.3628 LaSr2 Ga11 O20
1.3416 YAlO3 1.3630 KLa(MoO4 )2
1.3418 Bi4 Ge3 O12 1.3630–2 Sc2 SiO5
1.342 YVO4 [11.347, 376–383] 1.365 La2 Be2 O5
1.3420 CaAl4 O7 1.3657 KLa(MoO4 )2
1.3425 Ca(NbO3 )2 1.3665 SrAl4 O7
1.3425 YVO4 1.3675 LaF3
1.3425 PbMoO4 1.3680 SrAl4 O7
1.3425 CdF2 − YF3 1.3690 CeF3
1.3437 LuAlO3 1.3707 La3 Ga5.5 Nb0.5 O14
1.3440 NaLa(MoO4 )2 1.3710 CaAl4 O7
1.345 NdAl3 (BO3 )4 1.3730 La3 Ga5 GeO14
1.3475 CaWO4 1.3730 La3 Ga5 SiO14
1.3482 KLu(WO4 )2 1.3730 La3 Ga5.5 Ta0.5 O14
1.3485 KY(MoO4 )2 1.3745 LiNbO3
1.3493 Ca3 Ga2 Ge4 O14 1.3760 LaMgAll1 O19
1.35 KGd(WO4 )2 [11.384, 385] 1.386 YVO4 [11.377, 386]
1.3500 CdF2 − LuF3 1.3868 LaBGeO5
1.3505 CaF2 − ScF3 1.3870 LiNbO3
1.351 La2 Be2 O5 1.3885 CaWO4
1.351 KGd(WO4 )2 [11.353] 1.4150 Y3 Al5 O12
1.3510 KGd(WO4 )2 1.430 YAlO3 [11.387]
1.3510 La2 Be2 O5 1.44 SrGd4 (SiO4 )3 O
1.3510 Sr3 Ga2 Ge4 O14 1.4444 Y3 Al5 O12 [11.213, 387]
1.3512 YAlO3 1.486 Sc2 O3 [11.308]
1.3514 YAlO3
1.3520 CdF2 − GdF3 powers in the kilowatt range from one disc are possible.
1.3525 Ca2 Y5 F19 Further power scaling with several discs in the cavity is
1.3525 KY(WO4 )2 also possible [11.311].
1.3525 Lu3 Al5 O12
1.3532 Lu3 Al5 O12 Yb fiber laser. Fiber lasers present another approach for
1.3533 Y3 Al5 O12 the generation of high powers with diffraction-limited
1.3533 KLa(MoO4 )2 beam quality. Since the introduction of the double-clad
1.3533 KLu(WO4 )2 fiber more than two decades ago and with the recent
1.354 La2 Be2 O5 technological advances in the fields of fiber fabrication
1.3545 KY(WO4 )2
and beam-shaped high-power diode lasers, the perfor-
mance of diode-pumped fiber lasers has dramatically
1.3550 LiNbO3
improved. Today, fiber lasers can compete with their
1.3550 KLu(WO4 )2
corresponding bulk crystalline systems in certain appli-
1.3565 CaSc2 O4
cations, especially when fundamental-transverse-mode
1.3572 Y3 Al5 O12
continuous-wave (CW) laser operation at output powers
≈ 1.358 Y2 O3 in the milliwatt to kilowatt range is required.
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 649

Basic aspects of fiber lasers. The invention of the


double-clad fiber geometry and the holey fiber concept Yb3+ (4f 13) Hee HSB Hc
has accelerated the scaling of the output power and hence 2
F7/2 (8) 2
the success of high-power Er, Nd and Yb fiber lasers. F5/2
For more-detailed reading a comprehensive introduction 4f 1h 2
F (14)
to the field of rare-earth-doped fiber lasers can be found L=3
S = 1/2 2
in [11.388]. F5/2 (6) 2
F7/2

Part C 11.2
The choice of the fiber material involves a number
of considerations: The maximum phonon energy, envi- Fig. 11.54 Level scheme of Yb3+ : free-ion state (one 4f hole 4f1h ),
ronmental durability, the drawability and the rare-earth electron–electron interaction (Hee ), splitting by spin–orbit inter-
solubility. The maximum phonon energy of the glass action HSB , and crystal field Hc . Pump and laser transitions are
sets the overall infrared transparency range of the fiber indicated by arrows
and the multiphonon relaxation rates that influence the
quantum efficiency of radiative electronic transitions by 399]. When rare-earth ions are doped into these
nonradiative decay. The important physical properties glasses [11.400], the radiative transition probabili-
of the popular glasses used for optical fibers are shown ties, and therefore the absorption and emission cross
in Table 11.16. sections, are high as a result of the high (≈ 2.6) re-
fractive index and the high degree of covalency of
• Silicate glass. This glass is the most important ma- the glass. Small phonon energies of 300–450 cm−1
terial used for optical fiber production [11.388,389]. produce low rates of multiphonon relaxation for
However, the maximum phonon energy is high mid-infrared transitions. The low thermal conduc-
(≈ 1100 cm−1 ) and has so far limited the emission tivity (Table 11.16) is, however, an important factor
wavelength for infrared fiber lasers using this mater-
ial to approximately 2.2 µm [11.390]. Silica is robust
and fibers fabricated from this material involve the óabs (10–21 cm2)
very effective modified chemical vapor deposition 10
(MCVD) technique. Reducing the OH− content in Yb: YAG
Absorption at 300 K
the glass, which has two main absorption peaks
in the range 1.3–2.0 µm, reduces the background
5
absorption of fibers [11.391].
• Fluoride glass. These glasses, especially the
heavy-metal fluorides [11.392, 393], are used
as host materials for mid-infrared fiber lasers. 0
The most widespread fluoride fiber material is 850 900 950 1000 1050
Wavelength (nm)
ZBLAN [11.394] with a mixture of 53 mol % ZrF4 ,
20 mol % BaF2 , 4 mol % LaF3 , 3 mol % AlF3 , and Fig. 11.55 Absorption spectrum of Yb:YAG at 300 K
20 mol % NaF. Since it can be readily drawn into
single-mode optical fiber [11.395] it is particu-
larly important to mid-infrared fiber lasers [11.396] óem (10–21 cm2)
and allows for high infrared transparency up to 40
Yb: YAG
≈ 6 µm. Nonradiative decay by multiphonon relax- Emission at 300 K
ation, however, becomes significant for transitions at 30
wavelengths longer than ≈ 3 µm. In addition to mid-
infrared applications, ZBLAN is mostly also used 20
for upconversion fiber lasers which need metastable
intermediate pump levels with low multiphonon re- 10
laxation rates. An overview of the spectroscopic
properties of rare-earth ions doped into ZBLAN is 0
900 950 1000 1050 1100
given in [11.397]. Wavelength (nm)
• Chalcogenide glasses. Chalcogenides are composed
of the chalcogen elements S, Se and Te [11.398, Fig. 11.56 Emission spectrum of Yb:YAG at 300 K
650 Part C Coherent and Incoherent Light Sources

a) Pl (W) çopt (%)


Thin disc of Pump radiation Laser radiation
laser active medium 700 60

600 50
500
40
400
Part C 11.2

Multiple reimaging Resonator 30


Heat sink
of pump radiation mirror 300
Pl 20
200
b) Section 1 Section 2 çopt
Folding mirror 100 roc = 0.5 m 10
Section 2
2 0 0
8 3 0 200 400 600 800 1000 1200 1400
Pp (W)
5 6

4
Fig. 11.58 Output power and optical efficiency for a thin-
7
1 disc Yb:YAG laser using a single disc. (Pp = pump power,
Section 1 Pl = laser output power, ηopt = optical-optica efficiency)
Parabolic Thin laser disc Collimated Crystal and Parabolic
mirror with heat sink pump radiation focal plane mirror
(cladding pumped). The former method is less scalable
Fig. 11.57 (a) Thin-disc laser setup, (b) multiple-pass pump optics since it relies on the use of expensive high-beam-
for 16 passes quality pump sources because core areas are usually
< 100 µm2 . On the other hand, the larger cladding
to be considered in the design of chalcogenide- area (> 104 µm2 ) allows for high-power diode-array
based lasers. So far, the most important glasses pumping [11.408–411]. We will here describe the
are the sulfide glasses GaLaS (GLS) [11.401] and cladding-pumping technique, which is one of the
GeGaS [11.402] because of the reasonably high most important developments in high-power fiber-laser
rare-earth solubility. technology.

Fiber, pump and resonator geometries. As bulk lasers, • Fiber designs for cladding pumping. In the de-
fiber lasers can be operated continuous wave, pulsed sign of cladding pumping, the core of the fiber is
(including Q-switching) and mode-locked. These op- generally made to guide a single transverse LP01
eration modes have been investigated intensively for mode. The shape of the multimode pump cladding
the common laser transitions near 1 µm in Nd3+ and (Fig. 11.59), however, can be shaped with a num-
Yb3+ , and near 1.5 µm in Er3+ . However, the small ber of geometries. The pump cladding, which in
fiber diameter limits the peak power by the dam- turn is surrounded by a low-refractive-index trans-
age threshold intensity and, hence, crystalline lasers parent polymer or glass, provides a high numerical
in bulk geometries are mostly preferred when high- aperture (NA) of typically 0.3–0.55. Photonic crys-
energy short pulses are needed. In an analogous way tal structures can be also used to improve cladding
to the optical excitation of bulk gain media (see pumping [11.412] for the operation of fiber lasers
the section on longitudinal and transversal pump- at the multi-hundred-watt level. There are three
ing in this Sect. 11.2.2), doped optical fibers can be main double-clad-fiber layouts: circular, circular
either end pumped (core pumped) or side pumped with offset core, and rectangular, as shown schemat-

Table 11.16 Properties of popular fiber materials


Fiber material Max. phonon energy Infrared transparency Propagation losses Thermal conductivity
(cm−1 ) (µm) (λ at minimum) (dB/km) (W/Km)
Silica 1100 [11.403] < 2.5 0.2 (1.55 µm) 1.38 [11.404]
ZBLAN 550 [11.397] < 6.0 0.05 (2.55 µm) 0.7–0.8 [11.405]
GaLaS 425 [11.406] < 8.0 0.5 (3.50 µm) 0.43– 0.5 [11.407]
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 651

ically in Fig. 11.59. In the case of circular pump


cladding [11.53] a portion of the launched pump a) b) c) d)
light is skew to the fiber axis and produces an in-
ner pump beam caustic that never crosses the core.
Asymmetric configurations significantly improve
the pump beam absorption in the core [11.413, 414].
Double-clad pump schemes have been demonstrated

Part C 11.2
with holey or photonic crystal fibers [11.415]. In Jacket Outer cladding Pump cladding Core
such fibers single-mode guiding and very large mode
areas are possible [11.416]. Fig. 11.59a–d Principal double-clad fiber geometries which in-
• Fiber-laser resonators. Typical free-running fiber- clude (a) circular-shaped pump cladding with axially positioned
laser resonators are shown schematically in core, (b) circular-shaped pump cladding with off-axially positioned
Fig. 11.60. In the simplest resonator (Fig. 11.60a), core, (c) rectangular-shaped pump cladding and (d) D-shaped pump
the pump light passes through a dichroic mirror that cladding
is highly reflective for the oscillating laser light.
Fresnel reflection at the cleaved output end facet drawbacks of significant thermal and thermo-optical
of the fiber can provide sufficient feedback for laser effects. Its large surface-area-to-volume ratio means
oscillation, although with an output-coupler mirror that the heat generated in the core is dissipated ef-
at the output end of the fiber the optical efficiency fectively by radiation and convection from the outer
can be maximized. In an alternative arrangement, the surface of the fiber.
pump light can be launched into the output end of the
fiber (Fig. 11.60b). In order to scale the output power, High-power Yb fiber lasers. Yb-doped fiber-lasers
each end of the fiber can be pumped (Fig. 11.60c). have been operated at CW and average output pow-
Due to its geometry, the fiber provides potentially ers in excess of 10 W [11.421–426], in excess of
high pump- and signal-beam intensities without the 100 W [11.427–433] and above 1 kW [11.434]. Also,
a 30 µm Yb-doped large-mode-area fiber has been used
Table 11.17 Material and laser parameters of Yb:YAG for the amplification of Q-switched Nd:YAG pulses at
repetition rates between 3 and 50 kHz with average out-
Growth method Czochralski [11.417] put powers up to 100 W. Pulse energies as high as
Temperature (◦ C) 1930 [11.417]
Crucible Ir (Re) [11.417]
Yb-distribution coefficient 1.0 [11.417] a)
Max. doping level (%) ≤ 100 [11.417]
Structure Cubic [11.417] Pump Output
Space group Ia3d-O10h [11.417] Fiber
Heat conductivity (Wm−1 K−1 ) M
b)
Undoped YAG 11.0 [11.417]
Yb-doped (5%) 6.8 [11.417] M
Pump
RE-density (1021 cm−3 ) 14 [11.417]
Fiber
λlaser (nm) 1030 [11.417] M
Output
1050 c)
σem (cm2 ) at 1030 nm 19 × 10−21 [11.286]
M
20 × 10−21 [11.418] Pump Pump
21 × 10−21 [11.419] Fiber
σem (cm2 ) at 1050 nm 3 × 10−21 [11.286] Output M
σabs (cm2 ) at 969 nm 8.3 × 10−21 [11.286]
7.7 × 10−21 [11.419]
Fig. 11.60a–c Schematic diagram of resonators used for
σabs (cm2 ) at 941 nm 8.2 × 10−21 [11.286]
free-running fiber lasers with (a) a single-end co-
τrad (µs) 1040 [11.417]
propagating pump, (b) a single-end counter-propagating
951 [11.420] pump and (c) dual-end pumps. M represents a mirror
652 Part C Coherent and Incoherent Light Sources

4 mJ with diffraction-limited beam quality have been the Er absorption at these wavelengths is rather small,
obtained in this case [11.435]. because the absorption cross sections are in the or-
der of 1 to 2 × 10−20 cm2 (Figs. 11.62, 63). Doping
Yb3+ crystalline lasers. The properties and laser pa- levels higher than 1 to 2% are critical, because of
rameters of Yb:YAG are listed in Table 11.17. In the increased reabsorption losses and higher rates for en-
meantime, besides Yb:YAG, a lot of Yb-doped laser ergy transfer processes, which depopulates the upper
materials have been explored and tested in CW, Q- laser level (4 I13/2 , 4 I13/2 ) → (4 I15/2 , 4 I9/2 ). Therefore,
Part C 11.2

switched and mode-locked operation. Table 11.18 shows to keep the Er3+ concentration low but achieve higher
an overview of Yb-doped laser crystals. absorption, the usual approach is to codope the Er3+ -
doped laser material with Yb3+ , which can be very
Er lasers at 1.5 µm (4 I13/2 → 4 I15/2 ) efficiently pumped around 975–980 nm. Then, the en-
For many years Er3+ -doped materials have been ergy transfer process (2 F5/2 , 4 I15/2 ) → (2 F7/2 , 4 I11/2 )
widely investigated for laser applications in the spec- is exploited (Fig. 11.61). The main task for the
tral range around 1.6 µm [11.436]. This laser transition optimization of Er lasers around 1.55 µm is thus
(4 I13/2 → 4 I15/2 , see Er3+ energy-level scheme depicted to find the optimum concentration for both dopant
in Fig. 11.61) is used for eye-safe lasers for medicine, ions.
telecommunication, remote sensing and light detecting
and ranging (LIDAR). Suitable erbium-doped mater- Crystals. The absorption spectra of Er3+ :YVO4 for
ials for the 1.6 µm laser transition should be at first the 4 I15/2 → 4 I11/2 and 4 I15/2 → 4 I13/2 transitions
characterized by a high phonon energy, which en- are shown in Figures 11.62 and 11.63, respec-
ables fast depopulation of the pump level 4 I11/2 via tively [11.437]. The peak absorption cross section for
nonradiative decay in order to prevent excited-state the 4 I15/2 → 4 I11/2 transition around 970 nm is up to
absorption (ESA, I11/2 → H11/2 , S3/2 ) and upcon-
4 2 4 2 × 10−20 cm2 , for the 4 I15/2 → 4 I13/2 transition around
version UC1, (4 I11/2 , 4 I11/2 ) → (4 I15/2 , 4 F7/2 ) from 1500 nm cross sections are higher, approximately up
the 4 I11/2 level and to populate efficiently the 4 I13/2 to 4 × 10−20 cm2 . The emission spectrum is shown
upper laser level (Fig. 11.61). The second important in Fig. 11.63. The peak emission cross sections of
condition is that the ESA transition 4 I13/2 → 4 I9/2 the 4 I13/2 → 4 I15/2 emission in Er3+ :YVO4 are up
should not spectrally overlap with the range of to 2 × 10−20 cm2 , in the long-wavelength tail, where
stimulated emission
 around 1.6 µm and that the upcon- the laser oscillation occurs, the peak cross sections
version process UC2, (4 I13/2 , 4 I13/2 ) → (4 I9/2 , 4 I15/2 ) are around 0.5 × 10−20 cm2 . These values are typi-
is weak. Additionally, a significant splitting of the cal for Er3+ -doped crystals, e.g., the peak emission
ground-state multiplet is advantageous to achieve cross section around 1550 nm is 0.31 × 10−20 cm2 for
a quasi-four-level system. These conditions are best
fulfilled by Er3+ -doped glasses and fibers, which
are to date the most efficient lasers at this tran- E (103 cm–1)
sition. However, glasses suffer from poor thermal 4
F7/2 UC1
and mechanical stability, thus Er3+ -doped crys- 20 2
H11/2
4
talline matrices are still being intensively investigated S3/2
ESA
in order to find suitable crystals for this laser 15
4
F9/2
transition. ESA
4
For most applications of Er3+ -doped laser mater- I9/2 UC2 Energy transfer
4
ials, laser diodes operating in the wavelength range 10 I11/2
around 975 nm (the 4 I15/2 → 4 I11/2 transition) are used
4
as a pump source, thus enabling all-solid-state laser sys- I13/2 Wr Wnr ë pump =
tems. With Ti:sapphire pump lasers in general better 5 980 nm
ë pump = ëlaser =
laser results are obtained, however, the overall effi- 977 nm 1.6 µm

ciency is low. Another possible pump wavelength lies 0 4


I15/2
around 1.5 µm, i. e., directly into the upper laser mul-
Er 3+ Yb3+
tiplet. However, for this wavelength region high-power
laser diodes are not yet available, therefore usually Er– Fig. 11.61 Energy-level diagram of Er3+ and Yb3+ in
glass lasers as pump sources are used. In any case, a YVO4 crystal
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 653

Table 11.18 Yb3+ -doped laser crystals and laser transitions 2 F5/2 → 2 F7/2
Crystal λlaser (µm) Pump T (K) Output mode Ref.
BaCaBO3 F 1.034 TiS laser 300 p [11.440]
CaF2 : Na ≈ 1.046–1.048 Laser diode 300 ML [11.441]
1.051 Laser diode 300 Q-switch [11.441]
CaF2 : Nd 1.0336 Xe lamp 120 p [11.442]

Part C 11.2
1.030–1.055 TiS laser 300 CW [11.443]
Ca4 GdO(BO3 )3 - Laser diode 300 CW [11.444]
1.032 TiS laser 300 CW [11.445]
1.035–1.088 Laser diode 300 CW [11.446]
1.050 Laser diode 300 CW [11.446, 447]
1.050 TiS laser 300 CW [11.447]
1.082 TiS laser 300 CW [11.445]
1.082 Laser diode 300 CW [11.447]
Ca5 (PO4 )3 F 1.043 TiS laser 300 CW [11.448, 449]
Ca3 Sr2 (PO4 )3 F 1.046 TiS laser 300 CW [11.450]
Ca4 Sr(PO4 )3 F 0.985 TiS laser 300 CW [11.450]
1.046 TiS laser 300 CW [11.450]
1.110 TiS laser 300 CW [11.450]
Ca4 YO(BO3 )3 1.018–1.087 TiS laser 300 CW [11.451]
1.032 Laser diode 300 CW [11.452]
1.060 TiS laser 300 CW [11.453]
1.084–1.096 TiS laser 300 CW [11.454]
Gd3 Ga5 O12 1.039 Laser diode 300 Q-switch [11.455]
Gd3 Ga5 O12 : Nd 1.0232 Xe lamp 77 p [11.456]
Gd3 Sc2 Al3 O12 : Nd 1.0299 Xe lamp 77 p [11.457]
Gd2 SiO5 1.028–1.093 Laser diode 300 CW [11.458]
1.030–1.039 Laser diode 300 CW [11.459]
1.045–1.070 Laser diode 300 CW [11.459]
1.081–1.097 Laser diode 399 CW [11.459]
1.089 Laser diode 300 CW [11.460, 461]
1.090 Laser diode 300 CW [11.462, 463]
1.091–1.105 Laser diode 300 p [11.459]
1.094 Laser diode 300 CW [11.461]
GdVO4 1.015 Laser diode 300 CW [11.464]
1.015 TiS laser 300 CW [11.465]
1.015–1.019 Laser diode 300 CW [11.466]
1.026–1.031 Laser diode 300 CW [11.466]
1.029 Laser diode 300 CW [11.464]
1.029 TiS laser 300 CW [11.465]
1.040 Laser diode 300 CW [11.466]
1.045 Laser diode 300 CW [11.466]
(Gd, Y)2 SiO5 1.030–1.089 Laser diode 300 CW [11.458]
KGd(WO4 )2 1.026–1.044 Laser diode 300 CW [11.467]
1.030–1.051 Laser diode 300 CW [11.468]
1.031–1.0374 Laser diode 300 ML [11.469]
654 Part C Coherent and Incoherent Light Sources

Table 11.18 (continued)


Crystal λlaser (µm) Pump T (K) Output mode Ref.
KLu(WO4 )2 1.030 Laser diode 300 CW [11.470]
1.030 TiS laser 300 CW [11.470]
1.044 TiS laser 300 CW [11.471]
1.0435 Laser diode 300 CW [11.471]
Part C 11.2

KY(WO4 )2 1.026 Laser diode 300 CW [11.417]


1.026–1.042 Laser diode 300 CW [11.467]
1.030 TiS laser 300 CW [11.472]
1.048 Laser diode 300 ML [11.473]
≈ 1.028 Laser diode 300 ML [11.474]
1.030 Laser diode 300 CW [11.475]
0.987–1.051 Laser diode 300 CW [11.476]
KYb(WO4 )2 1.068 TiS laser 300 CW [11.477]
1.074 TiS laser 300 qCW [11.478]
LaSc3 (BO3 )4 1.044 TiS laser 300 CW [11.417]
1.045 TiS laser 300 CW [11.479]
0.995–1.087 Laser diode 300 CW [11.480]
LiGd(MoO4 )2 1.027–1.0335 Laser diode 300 CW [11.481]
LiNbO3 -waveguide 1.008 TiS laser 300 CW [11.482]
1.030 TiS laser 300 CW [11.482]
1.060 TiS laser 300 CW [11.482]
LiNbO3 : MgO 1.063 Laser diode 300 CW [11.483]
Li6 Y(BO3 )3 1.040 Laser diode 300 CW [11.484]
Lu3 Al5 O12 1.0297 Xe lamp 77 p [11.456]
1.03 Laser diode 175 CW [11.485]
Lu3 Al5 O12 : Nd, Cr 1.0294 Xe lamp 77 p [11.456]
Lu3 Ga5 O12 : Nd 1.0230 Xe lamp 77 p [11.456]
Lu2 O3 ≈ 1.029–1.038 TiS laser 300 ML [11.486]
1.032 Laser diode 300 CW [11.417]
ceramics 1.035 Laser diode 300 CW [11.487]
ceramics 1.079 Laser diode 300 CW [11.487]
Laser diode 300 CW [11.475]
Lu3 Sc2 Al3 O12 : Nd 1.0299 Xe lamp 77 p [11.457]
LuVO4 1.0347 Laser diode 300 CW [11.488]
1.041 Ti laser 300 CW [11.488]
1.0444 Laser diode 300 CW [11.488]
1.0527 Laser diode 300 CW [11.488]
NaGd(WO4 )2 1.016–1.049 TiS laser 300 CW [11.489]
1.023 TiS laser 300 CW [11.490]
1.033 Laser diode 300 CW [11.490]
NaLa(MoO4 )2 1.016–1.064 TiS laser 300 CW [11.491]
1.017 Laser diode 300 CW [11.492]
≈ 1.020 Laser diode 300 Q-switch [11.492]
1.023 Laser diode 300 CW [11.492]
1.035 Laser diode 300 CW [11.491]
NaLa(WO4 )2 1.017–1.057 TiS laser 300 CW [11.493]
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 655

Table 11.18 (continued)


Crystal λlaser (µm) Pump T (K) Output mode Ref.
Sc2 O3 1.041 TiS laser 300 CW [11.494]
1.0416 TiS laser 300 CW [11.495]
1.0946 TiS laser 300 CW [11.495]
ceramic 1.041 Laser diode 300 CW [11.496]

Part C 11.2
ceramic 1.094 Laser diode 300 CW [11.496]
Sr5 (PO4 )3 F 0.985 Cr:LiSAF 300 p [11.497]
0.985 TiS laser 300 CW [11.498, 499]
1.047 TiS laser 300 CW, qCW [11.500, 501]
Laser diode 300 p [11.502]
Sr5−x Bax (PO4 )3 F ≈ 1.048 TiS laser 300 CW [11.500]
(Sr0.7 Ca0.3 )3 Y(BO3 )3 Laser diode 300 CW, qCW [11.503]
Sr5 (VO4 )3 F 1.044 TiS laser 300 p [11.450]
Sr3 Y(BO3 )3 Laser diode 300 CW, qCW [11.494]
SrY4 (SiO4 )3 1.020–1.095 Laser diode 300 CW [11.504]
≈ 1.068 Laser diode 300 ML [11.504]
Y3 Al5 O12 1.016–1.095 TiS laser 300 CW [11.505]
1.0293 Xe lamp 77 p [11.456]
1.0296 Xe lamp 77 p [11.279]
1.023–1.052 Laser diode 300 CW [11.506]
1.029 Laser diode 300 CW, qCW [11.507]
waveguide 1.03 TiS laser 300 CW [11.508]
1.030 TiS laser 300 CW [11.509]
1.03 Laser diode 300 CW [11.280, 417,
507, 510]
1.03 Laser diode 300 Q-switch [11.511, 512]
1.03 Laser diode 300 ML [11.513]
1.03 TiS laser 300 Q-switch [11.514, 515]
waveguide 1.03 Laser diode 300 CW [11.516]
waveguide 1.03 Laser diode 300 CW [11.517]
waveguide 1.03 Laser diode 300 Q-switch [11.517]
1.031 Laser diode 300 p [11.501]
1.031 Laser diode 300 CW [11.518, 519]
≈ 1.0312 Laser diode 300 ML [11.519]
1.0494–1.0504 Laser diode 300 CW [11.520]
1.070 Laser diode 300 CW [11.311]
Y3 Al5 O12 : Nd 1.0297 Xe lamp 200 p [11.456]
waveguide 1.03 TiS laser 300 CW [11.521]
Y3 Al5 O12 : Nd, Cr 1.0298 Xe lamp 210 P [11.456]
YAl3 (BO3 )4 ≈ 1.040 Laser diode 300 CW [11.522]
1.120–1.140 Laser diode 300 CW [11.523, 524]
Y3 Ga5 O12 : Nd 1.0233 Xe lamp 77 P [11.456]
YLiF4 ≈ 0.991–1.022 Laser diode 77 P [11.525]
YLuSiO5 1.014–1.091 Laser diode 300 CW [11.526]
Y2 O3 ceramic ≈ 1.076 Laser diode 300 CW [11.527]
ceramic ≈ 1.076 Laser diode 300 ML [11.527]
ceramic 1.0767–1.0784 Laser diode 300 CW [11.520]
ceramic 1.078 Laser diode 300 CW [11.528]
656 Part C Coherent and Incoherent Light Sources

Table 11.18 (continued)


Crystal λlaser (µm) Pump T (K) Output mode Ref.
Y2 SiO5 1.000–1.010 Laser diode 300 CW [11.529]
1.082 Laser diode 300 CW [11.529]
Y3 Sc1.0 Al4.1 O12 ceramic ≈ 1.060 Laser diode 300 CW, ML [11.530]
YVO4 1.020–1.027 Laser diode 300 CW [11.531]
Part C 11.2

1.037 TiS laser 300 CW [11.532]


1.039 Laser diode 300 CW [11.532]

Er:YAlO3 [11.436], 0.33 × 10−20 cm2 for Er:Y2 SiO5 tioned loss mechanism of reabsorption and upconversion
[11.438], 0.45 × 10−20 cm2 for Er:YAG [11.436], already take place. The laser threshold is below 200 mW
0.42 × 10−20 cm2 for Er:YLF [11.436], and 0.59 × of incident power and below 100 mW of absorbed pump
10−20 cm2 for Er:LaGaO3 [11.439]. power.
From the absorption and emission spectra the gain These values for the slope efficiency, the laser thresh-
coefficient curves (Fig. 11.64) can be calculated by old and the output power are typical for well-performing
Er3+ -doped crystals, such as for Y3 Al5 O12 [11.533] and
g = N[Pσem − (1 − P)σabs ] , LaSc3 (BO3 )4 [11.534].
where N is the ion concentration and P is the inversion Recently, high-power and ultra-efficient laser op-
coefficient, defined as the ratio between the populations eration of an Er:YAG laser near 1645 nm with
in the 4 I13/2 and the 4 I15/2 levels. It can be seen that for approximately 60 W [11.535–538] of output power
Er3+ :YVO4 already for an inversion coefficient of P ≈ was demonstrated using a high-power fibre laser at
0.2 laser oscillation should be possible within a spectral 1532 nm as a pump source (so-called in-band pump-
range from approximately 1530 nm to 1610 nm. ing (Fig. 11.65b). This work demonstrates that the small
In Fig. 11.65a the input–output characteristics of Stokes shift between the pump and laser radiation
Ti:sapphire-pumped Er3+ :YVO4 crystals with 0.5% Er (1532 nm/1645 nm) yields very efficient Er lasers with
and 1% Er doping, operating at 1604 nm, are shown. slope efficiencies up to 80%.
The slope efficiency with respect to the incident power In Table 11.19 an overview of crystalline room-
is about 7–8%. It should be noted that with respect temperature Er3+ lasers is given. Note that lasers on
to the absorbed power the 0.5% Er:YVO4 crystal ex- the 4 S3/2 → 4 I9/2 transition are also listed.
hibits a higher slope efficiency. This indicates that for
the more highly doped sample (1% Er) the aforemen-
óabs , óem (1020 cm–2)
2
óabs (1020 cm–2) ó 4
I15/2 « 4I13/2
1,5 óabs
4
I15/2 ® 4I11/2 1 ðem
ó spectrum
ð spectrum
1 0
4
ð

0.5 2

0
1450 1500 1550 1600 1650 1700
0 Wavelength (nm)
970 980 990 1000 1010
Wavelength (nm)
Fig. 11.63 Spectra of absorption cross sections due to the
Fig. 11.62 Polarized absorption spectra at room tempera- 4I → 4 I13/2 transition of Er3+ in YVO4 crystal (dotted
15/2
ture of an Er3+ :YVO4 crystal in the spectral range of the lines) and emission cross sections (4 I13/2 → 4 I15/2 ) (solid
15/2 → I11/2 transition. (After [11.437]) lines) for σ and π polarization. (After [11.437])
4I 4
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 657

Glass. Laser oscillation in Er3+ -doped and Yb3+ ,Er3+ -


Gain coefficient g (cm–1)
codoped silicate and phosphate glasses was investigated
6
as early as the mid-1960s [11.539–541]. The three-level 4 ó
behavior of the Er3+ system and the weak absorp- 2
tion of pump radiation caused by the requirement 0
–2
of low dopant concentration (usually approximately P = 0.1; 0.2; 0.3; 0.4
–4
2 to 5 × 1019 cm−3 ) makes it difficult to obtain ef- –6
–8

Part C 11.2
ficient laser operation in singly Er3+ -doped glasses. –10
Therefore, Yb3+ codoping is necessary in order to 6 ð
absorb the pump light efficiently at wavelengths 4
2
around 1 µm. Continuous-wave laser oscillation, Q- 0
switched [11.542, 543] and quasi-CW operation with –2 P = 0.1; 0.2; 0.3; 0.4
pulse energies up to 35 J and average output pow- –4
–6
ers up to 20 W have been obtained [11.544–548]. –8
The pulse duration of the Xe flashlamps is sev- –10
1480 1500 1520 1540 1560 1580 1600 1620
eral milliseconds, thus matching the upper-laser-level Wavelength (nm)
lifetime of the Er3+ 4 I13/2 level. Also laser diodes
can be efficiently applied as pump sources. Wu Fig. 11.64 Gain coefficient curves derived for both polarizations for
et al. [11.549] used pulsed laser diodes in a transver- Er3+ :YVO4 in the spectral range of the 4 I15/2 → 4 I11/2 laser tran-
sal excitation scheme. Using a repetition rate of sition for four values of the inversion parameter P (larger gain
50 Hz, a pump pulse duration of 2.5 ms and a peak values for larger P). Arrows denote the wavelengths for which laser
pump power of ≈ 1.5 kW, an average output power oscillation was realized. (After [11.437])
of 8.5 W was obtained, corresponding to an out-
put energy of 170 mJ per pulse. A comparison and a) Pout (mW)
discussion of different pumping schemes is given 120
in [11.550]. In all experiments, the main problem 0.5 % Er: YVO4
of glass materials compared to crystals is the low 100 çabs = 19 %, çinc = 6.7 %

heat conductivity (for Kigre QE7 0.82 W/mK [11.547] 1 % Er: YVO4
80 çabs = 13 %, çinc = 8 %
versus 13 W/mK for YAG). Thus, the introduced
heating power and therefore also the extractable 60
output power and/or repetition rate is limited and
high-power continuous-wave excitation of Er3+ -doped 40
glasses is difficult. Despite this, the overall perfor-
mance of the Kigre QE7 and QX glasses is better than 20
that of Er3+ -doped crystals. Obaton et al. [11.551]
0
obtained a slope efficiency of 21% in a diode end- 0 500 1000 1500 2000
pumped setup for a QX glass. Diening [11.552] Pin (mW)
b) Output power (W)
compared Kigre QE7 glass with Er3+ :LaSc3 (BO3 )4
70
and Y3 Al5 O12 in the same setup (Fig. 11.66). The
achieved output power and slope efficiency for 60
the QE7 glass are about twice as high as for
50
Er3+ :LaSc3 (BO3 )4 .
40

Fig. 11.65 (a) Input–output curve of the CW laser oscil- 30


lation of Er3+ (0.5%):YVO4 crystal (λlaser = 1604 nm, 20
output mirror transmission = 1%). The slope efficiencies
are given with respect to the absorbed (ηabs ) and incident 10
(ηin ) power. (Results from [11.437]). (b) In-band pump- 0
ing of Er:YAG with a fiber laser at 1532 nm and lasing at 0 20 40 60 80
Incident pump power (W)
λlaser = 1645 nm [11.535]
658 Part C Coherent and Incoherent Light Sources

Table 11.19 Overview of room-temperature Er3+ -doped laser operating around 1.6 µm on the 4I
13/2 → 4 I15/2 and on the
4S
3/2 → 4 I9/2 transition
Crystal λlaser (nm) Transition Slope Mode of Pump source/Remarks Ref.
efficiency (%) operation
13/2 → I15/2
Ca2 Al2 SiO7 1530 nm 4I 4 1.1 CW Ti:Sapphire 940 nm, 975 nm [11.553]
13/2 → I15/2
1550 nm 4I 4 1.5 CW Ti:Sapphire 940 nm, 975 nm [11.553]
13/2 → I15/2
4I 4
Part C 11.2

1555 nm 5 CW Ti:Sapphire 940 nm, 975 nm [11.553]


LiNbO3 : Ti 1532 nm 4I
13/2 → I15/2
4 6 CW Tl:KCl, 1477 nm [11.554]
13/2 → I15/2
1563 nm 4I 4 3 CW, pulsed Tl:KCl 1479 nm, 1484 nm [11.555]
13/2 → I15/2
1576 nm 4I 4 CW, pulsed Tl:KCl 1479 nm, 1484 nm [11.555]
13/2 → I15/2
SrY4 (SiO4 )3 O 1554 nm 4I 4 0.4 CW Laser diode 980 nm [11.556]
YAlO3 1662 nm 4S
3/2 →4I
9/2 10.1 CW Kr+ [11.557]
3/2 → I9/2
1663 nm 4S 4 0.07 Pulsed Xe-flash lamp [11.558]
3/2 → I9/2
1663 nm 4S 4 Pulsed Xe-flash lamp [11.559,
560]
1663.2 nm 4S
3/2 →4 I9/2 Pulsed Xe-flash lamp [11.561–
563]
1663.2 nm 4S
3/2 → I9/2
4 CW Ar+ , 488 nm [11.564]
3/2 → I9/2
1667 nm 4S 4 0.02 Pulsed Xe-flash lamp [11.565]
1677.6 nm 4S
3/2 → I9/2
4 2.2 CW Ar+ , 488 nm [11.564]
3/2 → I9/2
1706 nm 4S 4 0.02 Pulsed Xe-flash lamp [11.565]
1706.1 nm 4S
3/2 →4I
9/2 CW Ar+ , 488 nm [11.564]
1729 nm 4S
3/2 →4I
9/2 0.02 Pulsed Xe-flash lamp [11.565]
1729.6 nm 4S
3/2 → I9/2
4 CW Ar+ , 488 nm [11.564]
LiYF4 1620 nm 4I
13/2 → I15/2
4 CW Kr+ , 647 nm [11.566]
1640 nm 4I
13/2 → 4I
15/2 CW Kr+ , 647 nm [11.566]
3/2 → I9/2
1664.0 nm 4S 4 Pulsed Xe flashlamp [11.567]
3/2 → I9/2
1730 nm 4S 4 0.6 Pulsed Xe flashlamp [11.568]
3/2 → I9/2
1732.0 nm 4S 4 Pulsed Xe flashlamp [11.569]
13/2 → I15/2
Y3 Al5 O12 1617 nm 4I 4 10 Q-switched (4 kHz) Er-fiber laser, 1543 nm [11.570]
13/2 → I15/2
1632 nm 4I 4 Pulsed Xe flashlamp [11.571]
13/2 → I15/2
1634 nm 4I 4 Pulsed, intracavity Er:glass 1549 nm [11.572]
1640 nm 4I
13/2 → I15/2
4 12.7 CW Kr+ , 647 nm [11.533]
13/2 → I15/2
1640 nm 4I 4 0,5 Q-switched Er:glass 1534 nm [11.573]
13/2 → I15/2
1644 nm 4I 4 7 Pulsed Er:glass 1535 nm [11.574]
13/2 → I15/2
1644.9 nm 4I 4 Pulsed Xe flashlamp [11.575]
13/2 → I15/2
1645 nm 4I 4 40 Pulsed Er:glass 1532 nm [11.576]
13/2 → I15/2
1645 nm 4I 4 40 Q-switched Yb, Er-doped fiber 1530 nm [11.577]
1645 nm 4I
13/2 → 4I
15/2 46 Pulsed 1.5 µm laser diodes [11.578]
1645 nm 4I
13/2 → 4I
15/2 40 CW Er-fiber laser, 1543 nm [11.570]
13/2 → I15/2
1645.3 nm 4I 4 81 CW, Q-switched Yb, Er-doped fiber 1530 nm [11.535]
13/2 → I15/2
1645.9 nm 4I 4 Pulsed Xe flashlamp [11.579]
1646 nm 4I
13/2 → 4I
15/2 7 CW laser diode [11.580]
3/2 → I9/2
1775.7 nm 4S 4 Pulsed Xe flashlamp [11.563,
571, 581]
Y3 Ga5 O12 1640 nm 4I
13/2 → I15/2
4 0.9 CW Kr+ , 647 nm [11.533]
Y3 Sc2 Ga3 O12 1643 nm 4I
13/2 → 4I
15/2 10 Pulsed Er:glass, 1532 nm [11.582]
Lu3 Al5 O12 1776.2 nm 4S
3/2 →4I
9/2 Pulsed Xe flashlamp [11.563]
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 659

Table 11.19 (continued)


Crystal λlaser (nm) Transition Slope Mode of Pump source/Remarks Ref.
efficiency (%) operation
3/2 → I9/2
KGd(WO4 )2 1715.5 nm 4S 4 Pulsed Xe flashlamp [11.583]
1732.5 nm 4S
3/2 →4I
9/2 Pulsed Xe flashlamp [11.583]
3/2 → I9/2
1733.0 nm 4S 4 Pulsed Xe flashlamp [11.584]
13/2 → I15/2

Part C 11.2
KY(WO4 )2 1540 nm 4I 4 1 CW Ti:Sapphire [11.585]
3/2 → I9/2
1737.2 nm 4S 4 Pulsed Xe flashlamp [11.584]
3/2 → I9/2
KLa(MoO4 )2 1730 nm 4S 4 Pulsed Xe flashlamp [11.586]
3/2 → I9/2
LiLuF4 1734.5 nm 4S 4 Pulsed Xe flashlamp [11.587,
588]
3/2 → I9/2
KLu(WO4 )2 1739.0 nm 4S 4 Pulsed Xe flashlamp [11.584]
3/2 → I9/2
KEr(WO4 )2 1737.2 nm 4S 4 Pulsed Xe flashlamp [11.584]
13/2 → I15/2
YVO4 1604 nm 4I 4 19 CW Ti:Sapphire [11.437]
(1531 nm,
1553 nm,
1564 nm,
1580 nm)
Y2 SiO5 1617 nm 4I
13/2 →4 I15/2 5.6 CW laser diode [11.580]
(1545 nm,
1567 nm,
1576 nm)
Sc2 SiO5 1558 nm 4I
13/2 →4 I15/2 CW Ti:Sapphire 979 nm [11.589]
1551 nm 4I
13/2 →4 I15/2 1.8 CW Ti:Sapphire 920 nm [11.589]
1551 nm 4I
13/2 →4 I15/2 2.4 CW laser diode 968 nm [11.589]
Sc2 Si2 O7 1545 nm 4I
13/2 →4 I15/2 2.6 CW Ti:Sapphire 980 nm [11.589]
1556 nm 4I
13/2 →4 I15/2 2.3 CW Ti:Sapphire 978 nm [11.589]
LaSc3 (BO3 )4 1563 nm 4I
13/2 →4 I15/2 6 CW laser diode 975 nm [11.534]
Ca4 YO(BO3 )3 1.5–1.6 µm 4I
13/2 →4 I15/2 26.8 CW laser diode [11.590,
591]
Ca4 GdO(BO3 )3 1.54 µm 4I
13/2 →4 I15/2 15 CW laser diode 975 nm [11.592]
7 Ti:Sapphire 902 nm

Fibers. Erbium-doped fiber lasers have been exten- of the 4 I13/2 level (8–10 ms) in silica fibers, despite
sively studied for their potential use as sources in the three-level laser character causing ground-state ab-
communication systems operation in the third com- sorption at this wavelength. Like in Er3+ -doped crystals
munication window around 1.55 µm. All these lasers and glasses, concentration quenching occurs. In order
oscillate on the 4 I13/2 → 4 I15/2 transition, either in to enhance the absorption efficiency without increas-
continuous-wave or pulsed mode. In singly Er3+ -doped ing the Er3+ concentration and/or fiber length, Yb3+
fibers, suitable pump wavelengths for using laser diodes codoping is used, especially when diode pumping be-
are 810 nm (4 I15/2 → 4 I9/2 ), 980 nm (4 I15/2 → 4 I11/2 ) tween 900 nm and 1000 nm is used. The requirement for
and 1480 nm (4 I15/2 → 4 I13/2 ). Other possible pump efficient operation is – as in the crystals and glasses – ef-
bands are around 660 nm (4 I15/2 → 4 F9/2 ), 532 nm and ficient energy transfer from the Yb3+ 2 F5/2 level to the
514.5 nm (4 I15/2 → 4 H11/2 ). The pump wavelengths at Er3+ 4 I13/2 level (Fig. 11.61). In Table 11.20, some of
810 nm and 514.5 nm suffer from strong excited-state the Er-fiber lasers around 1.55 µm are summarized. For
absorption, yielding a loss of pump photons [11.593]. a very detailed discussion of Er3+ -doped fiber lasers
The gain coefficient of Er-doped fibers is rather high and amplifier see [11.595]. In summary, Er3+ -doped
(11 dB/mW [11.594]) due to the fairly high peak emis- fiber lasers operating around 1.55 mm are extremely ef-
sion cross section of 4–7 × 10−21 and the long lifetime ficient. Output powers in the watt range are possible.
660 Part C Coherent and Incoherent Light Sources

Pout (mW)
11.2.4 Mid-Infrared Lasers
300
Basics
250 The mid-infrared wavelength range ≈ 1.9–5.0 µm is of
Kigre QE7 interest for a number of applications. Mid-infrared solid-
200 Yb, Er: La Sc3 (Bo3)4 state lasers serve as light sources for spectroscopy, e.g.,
Yb, Er: Y3 Al5 O12
in remote sensing of the atmosphere, as the frequencies
Part C 11.2

150 of internal vibrational motion of many molecules can be


found in this spectral region. Other applications include
100
medicine, e.g., microsurgery and dentistry in the region
50 of high water absorption around 2.7–3 µm. Laser wave-
lengths near 2 µm are suitable for tissue welding and
0 lithotripsy.
0 500 1000 1500 2000 2500 3000
Pin (mW) The first mid-infrared laser was operated in 1960,
shortly after the invention of the laser itself. It was op-
Fig. 11.66 Results of the laser experiments with Kigre QE7 erated at 2.6 µm in a calcium fluoride crystal doped
glass, Yb3+ (10%), Er3+ (0.5%): LaSc3 (BO3 )4 and Yb3+ , with trivalent uranium [11.608]. Pulsed excitation and
Er3+ (0.5%): Y3 AL5 O12 . (After [11.552]) cooling to low temperatures were typically required for
novel laser transitions in the early years. Two years later,
Nowadays up to 100 W of output power are commer- a Dy2+ -doped CaF2 laser at 2.36 µm was also demon-
cially available [11.596]. Most efficient pumping occurs strated in continuous-wave operation [11.609, 610].
at 1480 nm, here slope efficiencies close to the quantum Among the lasers based on trivalent rare-earth ions, the
limit of 95% are possible. Pumping at 980 nm is less transitions near 2 µm in Tm3+ and Ho3+ were operated
efficient due to the higher quantum defect, however, at in CaWO4 in 1962 [11.611,612]. The first observation of
this wavelength highly efficient and reliable high-power coherent emission near 3 µm from erbium ions was re-
laser diodes are available. ported in 1967 [11.613]. Since those early years, a large
number of new host materials has been developed and
Other near-infrared Er3+ lasers. Room-temperature various new laser transitions in the mid-infrared spectral
laser oscillation in Er3+ -doped crystals in the near- region have been demonstrated (for a comprehen-
infrared spectral range has also been observed at sive overview of ion–host combinations, see [11.614]).
other wavelengths. In Yb3+ -codoped Er3+ :YLiF4 an Around 1990, Tm3+ - and Ho3+ -doped solid-state laser
upconversion pumping scheme was realized for the systems in Y3 Al5 O12 (YAG), YLiF4 (YLF), YVO4 , and
3/2 → I11/2 transition at 1234 nm, which allowed
4S 4 Y3 Sc2 Ga3 O12 (YSGG) were shown to operate between
continuous-wave room-temperature Ti:sapphire- and 1.86 and 2.46 µm [11.615–618], and Er3+ -doped lasers
diode-pumped laser oscillation [11.597, 598]. Under in similar host systems cover the wavelength range of
Ti:sapphire excitation around 966 nm output powers 2.66–2.94 µm. Short-pulse lasers at these wavelengths
of 160 mW and slope efficiencies of up to 22% were have been demonstrated [11.619, 620].
obtained. Note, that without the Yb codoping, the out- Nowadays, mid-infrared laser transitions ranging
put powers were an order of magnitude lower. Under from 1.8 µm up to 7.2 µm [11.621] are known in di-
diode laser pumping at 966 nm, Yb3+ ,Er3+ :YLiF4 ex- valent Dy, trivalent Tm, Ho, Er, Dy, Pr, Tb, and Nd, as
hibited output powers of 80 mW and slope efficiencies well as in trivalent U. The current state of the art in solid-
of 7%. state lasers occurring in rare-earth ions such as Tm3+ ,
For this transition Xe flashlamp excitation is Ho3+ , Er3+ and others and their population mecha-
also possible allowing room-temperature laser oscil- nisms are discussed in this section on the basis of the
lation in YLiF4 [11.599–601], LuLiF4 [11.602] and spectroscopic properties of these ions. Continuous-wave
YAlO3 [11.603]. In BaYb2 F8 , the 4 F9/2 → 4 I13/2 transi- fundamental-mode power levels ranging from a few mW
tion at 1260 nm exhibited laser oscillation under pulsed near 4 µm up to ≈ 100 W near 2 µm have been demon-
Nd laser or Xe flashlamp excitation [11.604]. Laser os- strated in recent years. Power-scaling methods and their
cillation on the 4 F9/2 → 4 I11/2 transition was obtained limitations, the possibilities to optimize the population
around 1.96 µm in BaYb2 F8 [11.605–607] under pulsed mechanisms and increase the efficiencies of these lasers,
Nd laser and Xe flashlamp excitation. as well as the prospects of future mid-infrared lasers in
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 661

Table 11.20 Overview over Er3+ and Yb3+ :Er3+ -doped silica fiber lasers. λlaser : laser wavelength, λpump : pump wavelength, lfiber :
fiber length, Pthr : laser threshold, η: slope efficiency, Pout : output power, Ppump : pump power, Ref.: reference, (l): launched, (inc):
incident, (abs): absorbed, NA: not available. (After [11.595])
λlaser λ Pum p Er Yb lfiber Remarks Pthr η Pout max. Ppump Ref.
(nm) (nm) concen- concen- (m) (mW) (%) (mW) (mW)
tration tration
Ar+ pump

Part C 11.2
1566 514.5 35 ppm Er - 13 44 (l) 10 (l) 56 600 (l) [11.622]
1560 532 150 ppm - 1 Ring laser 10 (l) 5.1 (l) 1.8 45 (l) [11.623]
Er2 O3
1535 532 100 ppm Er - 15 Doubled NA 28 1000 3600 [11.624]
Nd:YAG
1560 806 500 ppm Er - 3.7 Laser diode 10 (l) 16 (l) 8 56 (l) [11.625]
1620 808 300 ppm Er - 1.5 Laser diode 3 (abs) 3.3 (abs) 0.13 7 (abs) [11.626]
1560 980 0.08 wt % - 0.9 Dye laser 2.5 (abs) 58 (abs) 4.7 11.3 (abs) [11.627]
1540 980 1100 ppm Er - 9.5 Ti:Sapphire > 10 (l) > 49 (l) 260 540 (l) [11.628]
1552 1460 1370 ppm Er - 5 2 laser diodes 37 (l) 14 (l) 8 93 (l) [11.629]
1552 1470 1370 ppm Er - 7 laser diode 44 (abs) 6.3 (abs) 1 60 (abs) [11.630]
1555 1480 45 ppm Er - 60 laser diode 6.5 (l) 38.8 (l) 3.3 15 (l) [11.631]
1560 1480 110 ppm - 42.6 laser diode 4.8 (abs) 58.6 (abs) 14.2 29 (abs) [11.632]
Er2 O3
1570 810 0.06 wt % 1.3 wt % 1.45 2 laser diodes 12.7 (l) 15.4 (l) 2.3 28 (l) [11.633]
1560 820 0.08% 1.7% 0.7 Dye laser 3.7 (abs) 7 (abs) NA NA [11.634]
1560 832 0.08% 1.7% 0.7 Dye laser 5 (abs) 8.5 (abs) NA NA [11.635]
1537 962 900 ppm 1.1% 1.6 laser diode 130 (l) 19 (l) 96 620 (l) [11.636]
1545 980 NA NA 0.07 laser diode 1 (abs) 25 (inc) 18.6 95 (inc) [11.637]
1535 1047 0.06% 1.8% 4 Nd:YLF 20 (l) 23 (l) 285 640 (l) [11.638]
1560 1064 0.08% 1.7% 0.91 Nd:YAG 8 (abs) 4.2 (abs) 1.3 (abs) 80 (abs) [11.634]
1535 1064 880 ppm 7500 NA Nd:YAG 37 (abs) 27 (abs) NA NA [11.639]
ppm
1545.6 980/1480 NA NA 0.07 Laser diode 10 (l) 50 (l) 166 340 (l) [11.640]

a number of rare-earth ions at transitions in the wave- this wavelength range will be discussed at the end of the
length range beyond 3 µm and extending to 5 µm are section.
described. Introductions to the fields of mid-infrared solid-state
The aspects relevant to rare-earth-ion-doped mid- crystalline and fiber lasers can be found in [11.641]
infrared solid-state lasers, such as the competition and [11.642], respectively.
between radiative and multiphonon decay and the con-
sequent choice of host materials for these wavelengths Decay mechanisms, host materials,
will be introduced next. The performance of the most and thermal issues
important mid-infrared laser transitions in the wave- Here a few fundamental aspects of lasers are discussed
length range 2–3 µm will then be discussed in detail: with emphasis on their impact on mid-infrared solid-
Tm3+ -doped lasers at 1.9 µm and 2.3 µm, Ho3+ -doped state lasers.
lasers at 2.1 µm and 2.9 µm, Er3+ -doped lasers at
2.7–2.9 µm, and Dy3+ -doped lasers at 2.9–3.4 µm. Radiative versus multiphonon decay. The choice of
At wavelengths beyond 3 µm, it becomes increasingly host material for mid-infrared solid-state lasers involves
difficult to find suitable host materials for actively a number of considerations. The maximum phonon
doped laser systems. This statement holds true for glass energy is the most important aspect. The optical trans-
fibers in the same way as for crystalline materials. The parency range relates to both the size of the bandgap
prospects for future mid-infrared solid-state lasers in and also the infrared absorption cut-off, hence to the vi-
662 Part C Coherent and Incoherent Light Sources

brational frequency ν of the anion–cation bonds of the


Multiphonon relaxation rate (s–1)
material. For an ordered structure,
1012
 
1 k 1011 Borate (1400 cm–1)
ν= , (11.89) 10 Posphate (1200 cm–1)
2π M 10
Silicate (1100 cm–1)
109
where M = m 1 m 2 /(m 1 + m 2 ) is the reduced mass for 8
Germanate (900 cm–1)
two bodies m 1 and m 2 vibrating with an elastic restoring 10 GLS (350 cm–1)
107
Part C 11.2

force k. The relative cation–anion bond strength is inti- Tellurite (700 cm–1)
10 6 ZBLA (500 cm–1)
mated by the field strength Z/r 2 , where Z is the valence
5
state of the cation or anion and r is the ionic radius. Gen- 10
erally, materials composed of large anions and cations 104
with low field strengths display high transparency in the 103
mid-infrared spectral region. 102
Radiative decay of excited states is in competition 101
2000 3000 4000 5000 6000 7000
with nonradiative multiphonon decay. The maximum Energy gap (cm–1)
phonon energy of the material sets the multiphonon re-
laxation rates, which influence the quantum efficiency. Fig. 11.67 Calculated and measured multiphonon relax-
The rate constant of a multiphonon relaxation process ation rates as a function of the energy gap between energy
decreases exponentially with the energy gap to the next levels for glasses with different maximum phonon energies.
lower-lying state and with the order of the process, i. e., (After [11.643, 644])
the number of phonons required to bridge the energy
gap [11.643, 646]. As an example, the multiphonon re- terials such as chlorides are required to ensure a long
9/2 lifetime in order to operate the 4.5 µm laser.
laxation rates for the common fiber glasses as a function 4I
of the energy gap between energy levels are shown in
Fig. 11.67. Host materials for mid-infrared lasers. Crystalline
The influence of multiphonon decay is stronger in oxide materials have been the laser host materials of
oxides than in fluorides because of the smaller atomic choice for several decades, as many oxide crystals are
mass m 2 of the anion and the larger elastic restoring comparatively easy to grow, environmentally stable,
force k (11.89), due to the stronger covalent bonds in ox- and possess high heat conductivities [11.647], frac-
ides [11.644], both resulting in larger maximum phonon ture limits, and refractive indices, the latter resulting
energies in oxides. Typically, nonradiative decay be- in large absorption and emission cross sections. Most
comes dominant if five or fewer phonons are required to prominent is Y3 Al5 O12 (YAG), together with other
bridge the energy gap [11.645]. Since an energy gap of
≈ 3300 cm−1 corresponds to a transition wavelength of
3 µm, radiative decay prevails for phonon energies below O2–, F –, Cl – O2–, F –, Cl –
4
≈ 600 cm−1 , which is roughly the maximum phonon I9/2 ô3 = 0.1 µs, 10 µs, 5 ms
Laser
energy of fluorides. Fluorides are, therefore, preferred 4.5 µm
4
over oxides as host materials for most mid-infrared laser I11/2 ô2 = 100 µs, 5 ms, 10 ms
transitions. Laser
In the example of Fig. 11.68, dominant laser (solid 2.8 µm
4
lines) and multiphonon (dotted lines) transitions from I13/2 ô1 = 5 ms, 10 ms, 15 ms
the three lowest-energy levels of Er3+ are indicated,
together with the corresponding lifetimes of the levels Laser
Pump 1.5 µm
in different classes of host materials. In high-phonon-
energy oxide host materials, only the 1.5 µm laser
transition possesses sufficiently high frequency and 4
I15/2
large energy gap, resulting in a long 4 I13/2 lifetime. Er 3+
On the other hand, the 4 I11/2 lifetime is significantly
quenched by multiphonon relaxation and the 2.8 µm Fig. 11.68 Radiative and laser (solid lines) versus nonradia-
laser originating in this level is more easily operated tive (dotted lines) decay of the lowest three excited states of
in fluoride host materials. Finally, low-phonon host ma- Er3+ in oxide, fluoride, and chloride host materials [11.645]
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 663

garnets, but in recent years materials such as mixed On the other hand, these materials provide phonon
garnets, the vanadates YVO4 and GdVO4 , the double energies in the range of 350–150 cm−1 [11.662]. Re-
tungstates KY(WO4 )2 and KGd(WO4 )2 , the sesquiox- cently, KPb2 Cl5 and related compounds have emerged
ides Y2 O3 , Sc2 O3 , and Lu2 O3 and others have shown as non-hygroscopic, hence promising candidates for
great promise for efficient lasing when doped with mid-infrared lasers [11.663–665]. Chalcogenide glasses
various rare-earth ions. Their performance decreases are composed of the chalcogen elements S, Se and
significantly when lasers are operated at wavelengths Te [11.666–668]. They are environmentally durable and

Part C 11.2
above ≈ 2.5–3 µm because of their high maximum have reasonably large glass-forming regions. When the
phonon energies (≈ 700–900 cm−1 ). Silicate glass is rare-earth ions are doped into these glasses [11.669],
perhaps the most important material used for optical the radiative transition probabilities and, therefore, the
fiber production [11.644, 648], however, in this material absorption and emission cross sections are high as a re-
the maximum phonon energy of ≈ 1100 cm−1 [11.649] sult of the high refractive index (≈ 2.6) of the glass
is even higher and has so far limited the emission wave- and the high degree of covalency of the rare-earth ion
length of mid-infrared fiber lasers using this material to with the surrounding medium. Maximum phonon en-
≈ 2.2 µm [11.650]. Silica is robust and involves the very ergies of 300–450 cm−1 [11.670] produce low rates
effective modified chemical vapor deposition (MCVD) of multiphonon relaxation (Fig. 11.67), and therefore
technique for fiber fabrication. Reducing the OH− con- high quantum efficiencies. The most important glasses
tent in the glass, which has two main absorption peaks are the sulfide glasses GaLaS (GLS) [11.671] and
in the range 1.3–2.0 µm [11.651], improves the near-to- GeGaS [11.672] because of the reasonably high rare-
mid-infrared utility. Rare-earth ions such as Nd3+ and earth solubility.
Er3+ which have high field strengths have low solubil- Studies into the use of ceramics as host mater-
ity in silicate glass, which can lead to clustering and ials for the rare-earths have recently made a lot of
microscale phase separation. progress [11.673]. These ceramics are composed of
The use of fluoride crystals and glasses as host ma- nanocrystallites of materials such as YAG and can
terials for mid-infrared solid-state lasers has found wide be produced in a simple cost-efficient process at rel-
acceptance. The heavy-metal fluorides [11.652,653] are atively low temperatures. This allows the fabrication
preferred as fiber materials, especially ZBLAN [11.654, of materials with very high melting points [11.674]
655], a mixture of 53 mol % ZrF4 , 20 mol % BaF2 , that are difficult to grow by other techniques such as
4 mol % LaF3 , 3 mol % AlF3 , and 20 mol % NaF. the Czochralski method. This class of materials is also
Since it can be readily drawn into single-mode optical available in a fiber geometry [11.675]. Ceramic fibers
fiber [11.656] it is particularly important to mid-infrared combine the characteristics of crystalline materials such
fiber lasers [11.657]. The large atomic weight of the as high absorption and emission cross sections, large
zirconium atom combined with relatively weak bond- thermal conductivity, and even the possibility of doping
ing provides a maximum phonon energy for ZBLAN with transition-metal ions [11.675] with the convenience
of ≈ 550 cm−1 [11.658] and allows for high infrared of guiding the pump and signal light in a fiber. While
transparency up to ≈ 6 µm. Multiphonon relaxation, bulk ceramics have already matured as laser host mater-
however, becomes significant for transitions at wave- ials, the losses of ceramic fibers are still comparatively
lengths longer than ≈ 3–3.5 µm. Compared to silica, high.
ZBLAN has a lower damage threshold. The crystal field
strength is also weaker [11.659]. An overview of the Specific aspects of operating mid-infrared lasers.
spectroscopic properties of rare-earth ions doped into As higher pump powers become available from laser-
ZBLAN is given in [11.658]. On the crystalline side, diode systems, it is generally recognized that thermal
the host materials LiYF4 , BaY2 F8 , and their respective and thermo-optical issues set limitations to the power
isostructural relatives have become the workhorses for scalability of end-pumped bulk laser systems. Owing to
many mid-infrared laser transitions [11.660, 661]. Be- the unfavorable temperature dependence of thermal and
cause of their fluoride content, these materials have to thermo-optical parameters [11.647], the large heat load
be grown under an atmosphere which excludes oxygen. in the crystal leads, firstly, to a significant temperature
Among the low-phonon host materials, many com- increase in the rod, secondly, to strong thermal lensing
pounds naturally possess low heat conductivity and are with pronounced spherical aberrations, and ultimately,
hygroscopic. This accounts for most of the halides, to rod fracture in a high-average-power end-pumped
with increasing hygroscopicity from chloride to iodide. system. Thermal management will be required when
664 Part C Coherent and Incoherent Light Sources

very high output powers are desired. In particular, for Thulium-doped solid-state lasers
high-power mid-infrared operation, thermal manage- at 1.9–2.0 µm and 2.3–2.5 µm
ment may be very important because of the decreased The use of the Tm3+ ion for mid-infrared solid-state
quantum efficiency and the consequently higher amount laser applications has been widespread, partly as a re-
of heat dissipation [11.676]. sult of the convenient absorption band near 0.79 µm,
Due to its geometry, the fiber provides potentially which allows for direct AlGaAs diode-laser pumping.
high pump and signal beam intensities without the draw- The primary luminescent transitions of Tm3+ relevant
Part C 11.2

backs of significant thermal and thermo-optical effects. to mid-infrared laser emission are the 3 F4 → 3 H5 tran-
Its large surface-area-to-volume ratio means that the heat sition at ≈ 2.3 µm and the 3 H4 → 3 H6 ground-state
generated from multiphonon relaxation in the core is transition at ≈ 1.9 µm; see the energy-level scheme in
dissipated effectively by radiation and convection from Fig. 11.69. The 3 F4 level is excited by the 0.79 µm pump
the outer surface of the fiber. This is especially true wavelength.
for single-clad, core-pumped single-mode fibers where
this ratio is highest [11.678]. The larger cladding area Three-level lasers at 1.9–2.0 µm. The first laser
(> 104 µm2 ) of double-clad fiber lasers allows for high- emission from Tm3+ ions was reported on the
power diode-array pumping [11.408, 679–682]. On the phonon-terminated 2 µm transition 3 H4 → 3 H6 in
other hand, double-clad fibers have a smaller surface- CaWO4 :Tm3+ in 1962 [11.611]. In 1975, pulsed
area-to-volume ratio and thermal issues need to be taken operation at room temperature was demonstrated
into account [11.683–685]. in Cr3+ -codoped YAG and YAlO3 [11.686]. Cr3+
While bulk crystalline mid-infrared lasers matured codoping allowed the experimentalist to improve the
already during the 1990s, the high costs of fabricating absorption of flashlamp or ion-laser pump light in
fibers with sufficiently low losses in the mid-infrared the visible spectral range by the active medium
region of the spectrum has impeded the necessary re- and subsequent energy transfer from Cr3+ to the
search efforts in the field of mid-infrared fiber lasers. Tm3+ lasing ions [11.687, 688]. The cross-relaxation
However, with the introduction of the double-clad fiber process (3 F4 , 3 H6 ) → (3 H4 , 3 H4 ) can transform one
and recent technological advances in the fields of pump photon absorbed in the 3 F4 or a higher-lying
fiber fabrication and beam-shaped high-power diode energy level into two excitations in the 3 H4 up-
lasers, the performance of diode-pumped fiber lasers per laser level of the 2 µm transition [11.616, 689]
has dramatically improved. Today, mid-infrared fiber (Fig. 11.69), thereby enhancing the quantum efficiency
lasers can compete with the corresponding bulk crys- of this laser by a factor of 2. Laser emission under
talline systems in certain applications, especially when diode pumping of the 3 F4 level at 780–790 nm was
fundamental-transverse-mode, CW laser operation at achieved in YAG in the late 1980s [11.690]. A single-
output powers in the milliwatt to the hundred watt range
is required.
3
A large number of techniques for pulsed operation F4 ô3 = 1.5 ms
including Q-switching and mode locking of fiber lasers Laser
have been explored. These techniques have been inves- 2.3 µm nr
tigated intensively for the common laser transitions at CR
1 µm in Nd3+ and Yb3+ , and at 1.5 µm in Er3+ , and 3
H5
are usually described in combination with these lasers. nr
3
The small fiber size limits the peak power through the H4 ô1 = 6.8 ms
damage-threshold intensity (propagating power per core
area) and, hence, crystalline lasers in bulk geometries or GSA Laser
optical parametric processes are often preferred when 2 µm
high-energy short pulses are needed. This argument ac-
3
counts especially for mid-infrared ZBLAN-based fiber H6
Tm3+
lasers, because these fibers possess a lower damage
threshold compared to silica fibers. The description of Fig. 11.69 Partial energy-level scheme of Tm3+ display-
mid-infrared fiber lasers is, therefore, confined to CW ing the measured lifetimes when doped into fluoride
operation and specific techniques for pulsed operation glass [11.677], NR and CR represent nonradiative decay
of fiber lasers are not discussed in this chapter. and cross-relaxation, respectively
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 665

frequency monolithic laser has also been reported in power under high-power diode side pumping [11.722],
YAG:Tm3+ [11.691]. and KY(WO4 )2 [11.723]. The latter laser has, as yet, not
Recently, 14 W, 18 W, and 36 W of output power shown a performance as good as for the same material
with high beam quality has been achieved with diode in bulk geometry [11.724] or in a waveguide geometry
pumping at room temperature in YAG:Tm3+ [11.692] but doped with Yb3+ and lasing at 1 µm [11.725]. Epi-
and in LiYF4 :Tm3+ in slab [11.693] and bulk [11.694] taxial layers of Tm:KLu(WO4 )2 /KLu(WO4 )2 have also
geometries, respectively. The latter approach could been operated with the laser cavity perpendicular to the

Part C 11.2
be scaled to 70 W, however currently with low layer in the 2 µm spectral range [11.726].
beam quality [11.695]. Two research groups reported The first explorations into fiber lasers utilizing
about 115 W and 120 W, respectively, of multi- the 1.9 µm ground-state transition related to the dye-
mode output power from diode-pumped YAG:Tm3+ laser pumping at 797 nm of a Tm3+ -doped silica
lasers [11.696, 697]. A microchip laser was demon- fiber laser [11.727]. Overlap of the main absorp-
strated in GdVO4 :Tm3+ [11.698]. A thin-disc laser has tion band with the emission wavelength of AlGaAs
also been demonstrated in YAG [11.699]. diode lasers quickly resulted in diode-laser pumping
The large degree of Stark splitting of the 3 H6 of these fiber lasers based on either silica [11.728]
ground state, combined with vibronic broadening of or fluoride [11.729] glass hosts. The cross-relaxation
the spectrum [11.700], provides the 3 H4 → 3 H6 tran- process (3 F4 , 3 H6 ) → (3 H4 , 3 H4 ) and enhancement of
sition with a very broad emission, spanning ≈ 400 nm excited ions in the 3 H4 upper laser level of the
in many hosts, which represents one of the broadest 2 µm transition (Fig. 11.69), is highly dependent on
luminescent transitions available from any rare-earth the overall concentration of Tm3+ ions and competi-
ion. Accordingly, its tunability is rather large, ranging tion from multiphonon relaxation from the 3 F4 level.
from 1.87–2.16 µm in YAG [11.701], 1.84–2.14 µm Although generally high concentrations of Tm3+ in
in YSGG [11.701], 1.93–2.00 µm in YAlO3 [11.702], low-phonon-energy glasses enable full exploitation of
1.93–2.09 µm in Y2 O3 [11.703], 1.93–2.16 µm in this beneficial process, it has been shown recently that
Sc2 O3 [11.703], 1.83–1.97 µm in CaF2 [11.704], this cross-relaxation process is resonant in a silica host
1.91–2.07 µm in LiYF4 [11.693], 1.85–2.06 µm in and hence only moderate (2–3 wt %) Tm3+ ion con-
BaY2 F8 [11.705], 1.86–1.99 µm in GdVO4 [11.706], centrations are required to maximize the benefits of
1.84–1.95 µm in LuVO4 [11.707], 1.79–2.04 µm cross-relaxation [11.730].
in KGd(WO4 )2 [11.708], and 1.81–2.03 µm in Also in fibers, the broad emission spectrum
NaGd(WO4 )2 [11.709]. As for many other transitions, allows a large degree of wavelength tunabil-
shifts in the center emission wavelength can be achieved ity [11.731]. Recently, tuning ranges of 230 nm
by substitution of host ions, e.g., from Y3 Al5 O12 to from 1.86–2.09 µm [11.732] and 250 nm from
Lu3 Al5 O12 [11.710]. The vanadate crystals GdVO4 and 1.72–1.97 µm [11.733] have been demonstrated. Since
YVO4 as well as double tungstates possess compara- the Tm3+ 1.9 µm transition can be favorably oper-
tively high absorption coefficients [11.698, 711, 712], ated in silica fiber (with its higher peak-power damage
allowing pumping also at 805–810 nm, where cheaper threshold compared to ZBLAN fiber), pulses in the
and more-reliable pump diodes than at 780–790 nm range of 190–500 fs have been obtained in additive-
are available. Exploiting the large gain bandwidth, pulse [11.734] or passive [11.735] mode-locking
mode-locked operation of Tm3+ 2 µm lasers with pulse arrangements using this broad emission spectrum. The
durations of 35 ps and 41 ps has been reported in smaller emission cross section and the three-level nature
YAG:Tm3+ [11.713] and YAG:Cr3+ ,Tm3+ [11.714], re- of the laser transition resulted in higher pump thresholds
spectively. Actively [11.715, 716] or passively [11.717] compared to standard Nd3+ -doped silica fiber lasers. Re-
Q-switched laser operation is useful in micro- absorption from the ground state of the Tm3+ ion has
surgery [11.718]. to be overcome because the ground-state multiplet is
Recent progress in the fields of crystalline epitax- the lower laser level. Reducing the population of the
ial growth and in-bulk refractive-index modification higher Stark levels of the ground state by cooling the
processes in glasses and crystals has enabled novel fiber causes emission at shorter wavelengths. Tunabil-
solid-state lasers in the waveguide geometry [11.719]. ity to longer wavelengths can be obtained by variation
As one of the results, Tm3+ waveguide lasers at of the fiber length because of the increased level of re-
2 µm have also been demonstrated in lead germanate absorption by the ground state with longer lengths of
glass [11.720], YAG [11.721] with up to 15 W of output fiber [11.736].
666 Part C Coherent and Incoherent Light Sources

Early power-scaling experiments involved the use Four-level lasers at 2.3–2.5 µm. The mid-infrared
of the convenient 1.064 µm YAG:Nd3+ laser which four-level CW laser at ≈ 2.3 µm on the transition
core-pumped the short-wavelength side of the 3 H5 3 F → 3 H has been operated in GSGG:Tm3+ and
4 5
level [11.737]. Pumping the long-wavelength side of the LiYF4 :Tm3+ , with wavelength tunability ranging from
3 H level with a high-power 1.319 µm YAG:Nd3+ laser 2.2–2.37 µm [11.748] and 2.2–2.46 µm [11.749], re-
5
also yielded efficient output [11.738]. In-band pump- spectively. This laser operates best at low Tm3+
ing of the transition at 1.57 µm in silica [11.739] and concentrations of < 2 at % in order to avoid the afore-
Part C 11.2

at 1.58–1.60 µm in fluoride glass [11.740, 741] has mentioned cross-relaxation, which in this case would
also been demonstrated. Whilst theoretical modeling of depopulate the upper laser level (Fig. 11.69). The life-
Tm3+ -doped silica fiber lasers [11.742] indicates that time of the lower laser level of the 3 F4 → 3 H5 transition
in-band pumping is the most efficient pump method is quite short and leads to a low pump threshold.
for silica-based fiber lasers because of the high Stokes Doping Tm3+ ions into a ZBLAN fiber offers an
efficiency, nevertheless, the wide availability of high- increased quantum efficiency of the 3 F4 level [11.750–
power AlGaAs diode lasers at 790–800 nm and the 752]. Deliberately designing the fiber to have a relatively
strong level of cross-relaxation in Tm3+ -doped silica low Tm3+ -ion concentration reduces cross-relaxation
means that such diode-cladding-pumped systems in both and hence severe lifetime quenching of the 3 F4 level.
standing-wave [11.736,743] and ring-resonator [11.744] The tunability extends from 2.25 µm to 2.5 µm [11.677].
arrangements are perhaps the most practical ways of Simultaneous lasing on the 3 H4 → 3 H6 transition at
producing high output power from this ion (Fig. 11.70). 1.9 µm produces a two-color fiber laser [11.753].
With Yb3+ sensitization and pumping at 975 nm, 75 W Applications requiring highly efficient output or multi-
of output power has been demonstrated [11.745]. Cur- mid-infrared-wavelength output will benefit from the
rently, the Tm3+ -doped silica fiber laser is the most use of Tm3+ -doped ZBLAN fibers.
mature of the mid-infrared fiber-laser systems pri-
marily because of the robustness and convenience Holmium-doped solid-state lasers at 2.1 µm
offered by the silica glass host. The maximum out- and 2.9 µm
put power from high-power Tm3+ -doped fiber lasers The use of the Ho3+ ion as the active dopant for
is now ≈ 85 W [11.743], which is comparable to the solid-state lasers opens up a number of very useful
equivalent diode-pumped Tm3+ -doped crystalline laser mid-infrared transitions. In this section, we will con-
systems [11.697]. centrate on the 5 I7 → 5 I8 ground-state transition at
≈ 2.1 µm and the 5 I6 → 5 I7 transition at ≈ 2.9 µm; see
the energy-level scheme in Fig. 11.71. One of the sig-
Output power (W) nificant shortcomings of Ho3+ , however, is the lack of
14 1.8 wt % Tm3+
12 3.6 mol % Tm3+, 0.4 mol % Ho3+ 5
S2
Laser
2.2 wt % Tm3+ 3.2 µm 5
10 F5
5
8 3 I4
F4
5
Laser I5
6
CR 3.9 µm 5
3
H5 I6
4 Laser
ET
3 2.9 µm
2 H4 5
I7
0
0 10 20 30 40 50 GSA Laser
Incident pump power (W) 2.1 µm

Fig. 11.70 Measured output powers from diode-cladding- 3 5


H6 I8
pumped fiber lasers using 1.8 wt % Tm3+ -doped sil- Tm3+ Ho3+
ica [11.735], 2.2 wt % Tm3+ -doped silica [11.746],
and 3.6 mol % Tm3+ , 0.4 mol % Ho3+ -doped fluoride Fig. 11.71 Partial energy-level scheme of Ho3+ with a Tm3+
glass [11.747] sensitizer. ET represents energy transfer
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 667

ground-state-absorption (GSA) transitions [11.754] that which provide an inhomogeneously broadened, and
overlap with convenient high-power pump sources. As therefore smoother, gain shape, a pulse duration as
a result, many of the early demonstrations of Ho3+ - short as 25 ps could be achieved [11.776]. Q-switched
doped room-temperature crystalline CW lasers [11.616] laser operation [11.781–783] has been investigated and
involved sensitizing with Tm3+ in order to access the applied for microsurgery [11.784].
convenient absorption bands and the practical cross- Besides the cross-relaxation and energy-transfer
relaxation process Tm3+ provides, as we have discussed processes shown in Fig. 11.71, several other energy-

Part C 11.2
in Sect. 11.3.1. Energy migration amongst the Tm3+ transfer processes can occur in Tm3+ ,Ho3+ -codoped
ions and a suitable Tm3+ :Ho3+ concentration ratio materials [11.785–789], thereby making the system
ensures that efficient energy transfer to Ho3+ takes rather complex and introducing parasitic processes
place [11.755, 756] (Fig. 11.71). which can deplete the Ho3+ 5 I7 upper laser level,
increase the laser threshold, and diminish the laser ef-
Three-level lasers at 2.1 µm. The 2 µm transition ficiency. Rather than codoping the host with Tm3+
5 I → 5 I in Ho3+ ions was first demonstrated as a laser ions and exciting the Ho3+ ions via nonradiative en-
7 8
in CaWO4 :Ho3+ in 1962 [11.612] and in Tm3+-codoped ergy transfer from the Tm3+ ions, one can directly
CaWO4 :Ho3+ in 1963 [11.757]. In 1971, pulsed op- pump the Ho3+ 5 I7 upper laser level at 1.9 µm using
eration at room temperature on this three-level laser laser diodes [11.790], the output from a 1.9 µm Tm3+
transition was demonstrated in LiYF4 [11.758]. CW laser [11.791], which provided up to 15 W [11.792] and
laser emission was achieved under Kr+ -laser pumping in 19 W [11.694] output power from Ho3+ , or a MgF2 :Co
Cr3+ ,Tm3+ -codoped YSAG:Ho3+ and YSGG:Ho3+ in laser [11.793]. This approach ensures a low quantum
1986 [11.759]. Like in 2 µm Tm3+ lasers (Sect. 11.3.1), defect and, hence, low heat generation in the laser crys-
the Cr3+ codopant served as a sensitizer for the ab- tal. This scheme was proven very successful by the use
sorption of pump light in the visible spectral range and of a high-power Tm3+ fiber laser as the pump source,
excitation of Tm3+ ions by energy transfer. The subse- providing 6.4 W of output power and a slope efficiency
quent excitation of Ho3+ ions by energy transfer from of 80% versus incident pump power at 1.9 µm [11.794].
Tm3+ [11.760, 761] profits from the same Tm3+ -Tm3+ Also an efficient 2 µm Ho3+ single-frequency ring laser
cross-relaxation as described for 2 µm Tm3+ lasers in has been demonstrated in this way [11.795].
Sect. 11.3.1 (Fig. 11.71). In the 1980s, laser emission The first fiber laser configuration making use of
at 2.1 µm in Ho3+ under diode pumping of the Tm3+ this transition employed ZBLANP glass (a variant of
3 F level at 780–790 nm with pump thresholds as low ZBLAN) and argon-ion pumping [11.796]. A year later,
4
as 5 mW was achieved in YAG [11.762–764]. Com- this was followed by the demonstration of an argon-ion-
pact, monolithic, low-threshold laser devices can be pumped Ho3+ -doped silica fiber laser [11.797]. In both
achieved in this way [11.765]. Besides many differ- cases, the fiber was singly doped with Ho3+ , the out-
ent garnet crystal systems, LiYF4 also regained interest put power < 1 mW, and each needed a relatively high
as a host material for CW diode-pumped 2 µm Ho3+ pump power to reach laser threshold. Improvements in
lasers around 1990 [11.766, 767]. An Yb3+ -codoped, the output power and efficiency have been made recently
diode-pumped Ho3+ laser at 2.1 µm has also been with Yb3+ -doped silica fiber laser pumping of the 5 I6
demonstrated [11.768]. Noise suppression [11.769,770], level [11.798]; however, the output power had only in-
amplitude and frequency stabilization [11.771–773] of creased to 280 mW because the pump fiber laser was
2 µm Ho3+ lasers have been investigated. operated at the low-efficiency 1150 nm wavelength. Us-
Attempts to exploit the rather large gain band- ing the pump wavelength of 1100 nm, which is more
width of Ho3+ near 2.0–2.1 µm by tuning the emission optimal with respect to the operation of an Yb3+ -doped
wavelength were reported in the early 1990s [11.774, silica fiber laser, the output power has been increased by
775]. Nowadays, tuning ranges of > 80 nm are approximately an order of magnitude [11.799].
achieved in host materials such as mixed YSGG:GSAG As mentioned above, a practical method of ef-
[11.776], BaY2 F8 :Ho3+ [11.777], and KYF4 [11.778]. ficiently generating laser emission on the 5 I7 → 5 I8
Mode-locking experiments have resulted in 800 ps, transition is to codope Ho3+ laser ions with Tm3+ sen-
370 ps, and 70 ps pulse durations, obtained in sitizer ions. The first demonstration of a fiber laser
YAG:Cr3+ ,Tm3+ ,Ho3+ [11.714], LiYF4 :Tm3+ ,Ho3+ operating with the Tm3+ ,Ho3+ system occurred in
[11.779], and BaY2 F8 :Tm3+ ,Ho3+ [11.780], respective- 1991 [11.800] when 250 mW was generated at a slope
ly. In mixed crystals of YSGG:GSAG:Cr3+ ,Tm3+ ,Ho3+ , efficiency of 52% from a Ti:sapphire-pumped fluoride
668 Part C Coherent and Incoherent Light Sources

fiber laser. A year later [11.801], this work was followed pumped crystalline lasers for the generation of 2.9 µm
by an increase in the Tm3+ concentration to improve output [11.809]. Recent reports on this transition include
cross-relaxation and resulted in a higher slope efficiency laser investigations of YAlO3 :Ho3+ [11.810], diode-
being obtained. Demonstration of a Tm3+ ,Ho3+ -doped pumped Yb3+ -codoped YGSS:Ho3+ with 10 mJ output
silica fiber laser soon followed [11.802, 803]; how- energy [11.811], and Cr3+ ,Yb3+ -codoped YGSS:Ho3+
ever, owing to lower Tm3+ concentrations which forces tunable in the range 2.84–3.05 µm [11.812] and in Q-
weaker cross-relaxation, significantly lower slope ef- switched operation [11.813]. Since the 5 I7 lower laser
Part C 11.2

ficiencies were measured, especially when pumped at level is a metastable excited state with a longer lifetime
1.064 µm [11.804]. When the concentrations are in- than the 5 I6 upper laser level, it is difficult to achieve
creased and the double-clad pump arrangement used, CW inversion on this transition. Cascade lasing on the
a significant augmentation of the output power to 5 I → 5 I and 5 I → 5 I transitions at 3 and 2 µm, re-
6 7 7 8
5.4 W has been demonstrated [11.805]. To date, the spectively [11.814, 815], may help to deplete the 5 I7
highest output power of 8.8 W from a fiber laser operat- level radiatively, i. e., without significant heat genera-
ing on the 5 I7 → 5 I8 transition has been produced by tion. Passive Q-switching of this transition has also been
a diode-cladding-pumped Tm3+ ,Ho3+ -doped fluoride demonstrated [11.813].
fiber laser [11.747] (Fig. 11.70). In an analogous way The combined effect of the infrared absorption
to recent demonstrations in bulk laser systems, tandem- cut-off wavelength of ≈ 2.5 µm for pure silica glass
pumping Ho3+ with a separate Tm3+ laser operating and the strong multiphonon relaxation quenching of
at 1.9 µm may also prove effective in fibers, because it mid-infrared transitions of rare-earth ions in this host
similarly exploits the cross-relaxation process between means that four-level fiber lasers operating on the
Tm3+ ions but avoids any ETU between Ho3+ ions in 5 I → 5 I transition at ≈ 2.9 µm have only involved
6 7
the 5 I7 upper laser level and excited Tm3+ ions [11.789]. fluoride glass as the host material. The first demon-
When sensitizing with Yb3+ ions, a Ho3+ -doped silica stration of a fiber laser using this transition [11.816]
fiber laser at 2.1 µm has been shown [11.806] to operate produced only ≈ 13 mW when pumped at a wavelength
at moderate efficiency levels despite the fact that the en- of 640 nm. High-power cascade lasing at 2.9 µm and
ergy transfer from Yb3+ to Ho3+ is quite nonresonant 2.1 µm has been employed to extend the output power
(Fig. 11.72). to 1.3 W [11.817] by removing bottlenecking at the 5 I7
level [11.807] via the second laser transition at 2.1 µm.
Four-level lasers at 2.9 µm. Laser emission at the In an analogous manner to the Er3+ -doped fluoride
transition 5 I6 → 5 I7 near 3 µm in an Ho3+ -doped crys- glass system discussed below, the most successful ar-
tal was demonstrated in 1976 [11.808]. Sensitizing rangement to date for extracting high power from this
Ho3+ with Yb3+ ions (see the energy-level scheme transition has involved the use of Pr3+ as a desensi-
in Fig. 11.72) in order to exploit the more-favorable tizer for the 5 I7 energy level: a maximum output power
absorption features of Yb3+ has been used in diode- of 2.5 W was produced when the pump wavelength
of 1100 nm from a Yb3+ -doped silica fiber laser was
used [11.818].
ET
5
I5 An Yb3+ -sensitized Ho3+ -doped ZBLAN fiber
2
F5/2 could be directly pumped with diode lasers and may
5
I6 efficiently provide high-power 2.9 µm output without
ô2 = 3.5 ms Laser the costly requirement of an intermediate laser system.
2.9 µm
GSA 5 Initial spectroscopic results look encouraging [11.819],
I7
ô1 = 12 ms however, the many excited ion interactions that a fluoride
Laser host provides may be problematic. A recent demonstra-
2.1 µm tion has shown that ion–ion interactions (specifically
ETU) in Ho3+ -doped fluoride glass are critical to the
2 5
production of 2.9 µm output from singly Ho3+ -doped
F7/2 I8
fluoride glass fiber lasers [11.820].
Yb3+ Ho3+

Fig. 11.72 Partial energy-level scheme of Ho3+ with Yb3+ Erbium-doped solid-state lasers at 2.7–2.9 µm
sensitizer displaying the measured lifetimes of Ho3+ when For a long time, the development of erbium lasers op-
doped into fluoride glass host [11.807] erating on the 4 I11/2 → 4 I13/2 transition near 3 µm was
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 669

dominated by crystalline systems. The early success of


the erbium 3 µm crystal laser has given rise to a signifi- a) b)
4 –17 3 –1
F7/2 W (10 cm s ), Ratio
cant amount of spectroscopic investigations. This has led 2 10
H11/2
to a deep understanding of the rather complex population 4
S3/2 9
mechanisms of this laser system and to the development ETU2 CR 8 W11
of a large number of suitable host materials. 4 7 W22
F9/2
6 Ratio
5

Part C 11.2
Crystalline lasers. The first observation of coherent 4
ETU1
I9/2 4
emission near 3 µm from erbium ions was reported 3
4 Laser
in 1967 [11.613]. Yttrium aluminum garnet (YAG) I11/2 2
was demonstrated as a host for the erbium 3 µm ETU2
1
laser [11.822] in 1975. In 1983, the first CW lasing near 0
4
I13/2 0 5 10 15
3 µm was obtained in this material [11.823]. At about 20 –3
Erbium concentration (10 cm )
the same time, it was established [11.824–827] that en-
ergy transfer processes [11.828] between neighboring Pump ETU1 CR
erbium ions in the host lattice play an important role
in this laser system. Energy transfer processes can be- 4
I15/2
come very efficient at high excitation density [11.829] 3+
Er
and govern the population mechanisms of the 3 µm
laser at high erbium concentration. In the energy-level Fig. 11.73 (a) Partial energy-level scheme of erbium indicating the
scheme of Fig. 11.73a, the important ETU and cross- pump and laser transitions, ETU1 from 4 I13/2 , ETU2 from 4 I11/2 , and
relaxation processes are introduced. The ETU process cross-relaxation (CR) from the thermally coupled 4 S3/2 and 2 H11/2
(4 I13/2 , 4 I13/2 ) → (4 I15/2 , 4 I9/2 ) leads to a fast deple- levels. (b) Macroscopic parameters of ETU1 from 4 I13/2 (W11 ) and
tion of the lower laser level and enables CW operation ETU2 from 4 I11/2 (W22 ) and the ratio W11 /W22 in ZBLAN:Er3+
of a laser transition which, otherwise, could be self- bulk glasses. (After [11.821])
terminating owing to the unfavorable lifetime ratio of
the upper compared to the lower laser level. The ETU given by [11.831]
process from 4 I13/2 can be so dominant that even under  
direct pumping of the 4 I13/2 lower laser level and subse- ln(1 − T ) b21 W22
ηsl = ηSt 2− 2 ,
quent excitation of the 4 I11/2 upper laser level by ETU, ln[(1 − T )(1 − L)] b2 W11
3 µm laser operation was demonstrated in several host (11.91)
materials [11.830].
This ETU process offers another great advantage. with T the transmission of the out-coupling mirror, L
Half of the ions that undergo this process are upcon- the internal resonator losses, and bi and Wii , the Boltz-
verted to the 4 I9/2 level and, by subsequent multiphonon mann factors and ETU parameters of the upper (i = 2)
relaxation, are recycled to the 4 I11/2 upper laser level and lower (i = 1) laser levels, respectively. If ETU oc-
from where they can each emit a second laser photon, curs only from the lower laser level, i. e., W22 = 0, we
for a single pump-photon absorption. For a large number obtain the predicted factor of two increase in slope ef-
of ions participating in this process, a slope efficiency ficiency from (11.91). The slope efficiency is reduced,
ηsl of twice the Stokes efficiency ηSt = λpump /λlaser however, by the resonator losses, the imperfect mode
is obtained [11.831], because the quantum efficiency overlap, and the ETU process from the upper laser level
ηQE = n laser /n pump of pump photons converted to laser in the case of W22 > 0. In the investigated host mater-
photons increases from 1 to 2 (λ and n are the ials, the parameters Wii of both ETU processes increase
wavelengths and photon numbers of laser and pump with increasing erbium concentration because of the in-
transitions, respectively): fluence of energy migration within the erbium 4 I11/2 and
4I
13/2 levels on ETU. The slope efficiency of (11.91) is
ηsl = ηQE ηSt = 2ηSt . (11.90) optimum for a maximum ratio W1 /W2 . Spectroscopy of
these processes in crystal hosts and laser experiments
This is illustrated in Fig. 11.74. revealed that the maximum ratio is obtained at dopant
In a simple rate-equation system which includes the concentrations of ≈ 12–15% in BaY2 F8 [11.832, 833],
processes shown in Fig. 11.73a the slope efficiency is ≈ 15% in LiYF4 [11.661], ≈ 30% in YSGG [11.834],
670 Part C Coherent and Incoherent Light Sources

pared to fluoride host materials because of the larger


4
F9/2 maximum phonon energies in oxides. With an energy
gap between the 4 I11/2 upper and 4 I13/2 lower laser lev-
100 % 50 % 25 % 13 % = çpump els of ≈ 3400–3500 cm−1 , the radiative decay becomes
4
I 9/2
dominant for phonon energies below ≈ 550 cm−1 . Since
4
I11/2 a long lifetime of the 4 I11/2 upper laser level provides
a small pump threshold, fluorides are preferable host
Part C 11.2

Laser materials [11.843] for this laser transition if the pump


4
I13/2 power is not many times above threshold.
1.0 1.5 1.75 1.83 ... 2 = çQE In the 1980s and 1990s, numerous host materials
were investigated for CW and pulsed laser operation of
GSA ETU1 ETU1 ETU1 Er3+ in the 2.7–2.9 µm region. A major role was played
by the family of garnet crystals YAG, YSGG, YSAG,
YGG, and GGG [11.615, 844, 845]. In the early years,
4
I15/2 Cr3+ codoping was used in order to improve the absorp-
Er3+
tion of broadband flashlamp pump light in the visible
Fig. 11.74 Partial energy-level scheme of erbium illustrat- spectral range and transfer the absorbed energy from
ing the process of energy recycling from the lower to Cr3+ to Er3+ . Typical output characteristics obtained
the upper laser level by ETU. Indicated are the relative were 2.7 W average power at a pump energy of 5 J with
pump rate ηp of the upper laser level and the quantum effi- a repetition rate of 10 Hz [11.845]. Doping levels up to
ciency ηQE which increases from 1 to 2 if a large number 100% substitution of Y3+ by Er3+ were tested [11.846].
of ions participate in the process. (After [11.836]) A new class of host materials, fluoride crystals such as
LiYF4 , BaY2 F8 , and others, became of importance in
and ≈ 50% in Y3 Al5 O12 [11.835]. A trend in this se- the late 1980s [11.847–850]. Laser thresholds as low
ries is the increase of the optimum erbium concentration as 5 mW were obtained under CW excitation by diode
with phonon energy of the host material. lasers [11.849].
Energy recycling by ETU is the most efficient In recent years, researchers have obtained CW and
way to operate a CW erbium laser near 3 µm. The quasi-CW diode-pumped output power levels exceeding
highest slope efficiency obtained experimentally is cur- 1 W at 3 µm from fluoride [11.661] and oxide [11.851–
rently 50% in LiYF4 :15% Er3+ [11.837]. The pump 853] crystalline host materials. A significant problem in
wavelength that provides the highest Stokes efficiency the energy-recycling regime is increased heat genera-
of ηSt = λpump /λlaser = 35% is 980 nm, which cor- tion due to the multiphonon relaxation 4 I9/2 → 4 I11/2
responds to pumping directly into the upper laser that follows each ETU process from the lower laser
level [11.838] (Fig. 11.73a). The highest slope efficiency level [11.676]. Glass bulk materials [11.854] suffer from
obtained experimentally [11.837] is currently ηsl = 50% the same thermal and thermo-optical drawbacks as the
in LiYF4 :15% Er3+ . This result shows that energy re- crystalline bulk materials, with even decreased thermal
cycling is indeed efficient and that slope efficiencies conductivity in the glass. A possible solution is diode
far above the Stokes efficiency can be obtained under side pumping, which leads to lower excitation den-
CW pumping. Under quasi-CW excitation, the slope ef- sities and correspondingly weaker ETU processes, as
ficiency is strongly reduced [11.839], because the lower well as better heat removal in the slab geometry. The
laser level is much less populated than in the steady- highest output powers of 1.8 W and later 4 W from an
state regime and ETU is less efficient [11.840, 841]. erbium 3 µm crystal laser [11.855, 856] have been ob-
Other operational regimes which deplete the lower laser tained in this way. A reduced erbium concentration with
level without recycling the energy to the upper laser correspondingly smaller parameters of the ETU pro-
level are less efficient. Consequently, neither co-lasing cesses may aid this approach. However, the efficiency
at the 1.6 µm transition from the lower laser level to the of the energy-recycling regime cannot be reached in this
ground state [11.842] nor energy transfer from the er- approach.
bium lower laser level to a rare-earth codopant [11.660] Other special configurations include the operation
have reached the efficiency of the recycling regime. of Er3+ -doped YAG, GGG, and YSGG lasers in mono-
Lifetime quenching of the 4 I11/2 upper laser level lithic cavities with output powers up to 0.5 W and
by multiphonon relaxation is stronger in oxide com- tunable single-frequency output [11.857] as well as mi-
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 671

crolasers in YSGG [11.858]. Pulsed output at 3 µm has see the measured GSA and ESA cross sections in
been generated from erbium-doped crystalline mater- Fig. 11.75a. Depletion of the lower laser level by ESA
ials in many configurations and regimes, e.g., under favorably results in a redistribution of its population den-
quasi-CW pumping [11.839, 841], active [11.859–868] sity and overcomes the bottleneck that results from the
and passive [11.869–872] Q-switching, and mode- long lower-level lifetime. However, slope efficiencies
locking [11.619, 869, 873]. obtained in this way were < 15%. Moreover, satura-
tion of the output power at 2.7 µm was observed and

Part C 11.2
Fiber lasers. The erbium-doped fluoride fiber represents the highest reported output powers were in the 20 mW
a promising alternative for the construction of a com- region [11.887, 888]. The excitation of the metastable
3/2 level (lifetime ≈ 580 µs [11.821]) led to inversion
pact and efficient all-solid-state laser emitting at the 4S
transition at 3 µm. Due to its geometry, the fiber pro- with respect to the 4 I13/2 level. A second laser transi-
vides large flexibility and potentially high pump and tion at 850 nm repopulated the 4 I13/2 lower laser level of
signal beam intensities without the drawbacks of ther- the 2.7 µm transition (Fig. 11.75b), causing the 2.7 µm
mal and thermo-optical effects. The first erbium 3 µm laser to saturate at low output powers [11.885]. Sig-
fiber laser was demonstrated in 1988 [11.875]. Single- nificant improvement in the performance of this laser
mode [11.876] and diode-pumped [11.877] operation system was obtained by deliberately operating a third
were demonstrated shortly afterwards. Although the life- laser transition 4 S3/2 → 4 I9/2 at 1.7 µm, thereby sup-
time of the 4 I13/2 lower laser level exceeds that of the pressing the competitive laser at 850 nm and recycling
4I
11/2 upper laser level, CW lasing can be obtained the excitation energy accumulated in the 4 S3/2 level into
on this four-level-laser transition in ZBLAN (but also the upper laser level; see the energy-level scheme in
in fluoride crystals, see the paragraph on crystalline Fig. 11.75b. The slope efficiency of the 2.7 µm transi-
lasers) without employing special techniques to depop- tion increased significantly to 23% [11.889], close to the
ulate the 4 I13/2 lower laser level, because the lower Stokes efficiency limit of 29% under 800 nm pumping.
laser level is not fed significantly by luminescent de- An output power of 150 mW was demonstrated ex-
cay or multiphonon relaxation from the upper laser perimentally [11.889]. Also a three-transition-cascade
level [11.878]. In addition, the Stark splitting of the laser
levels contributes to population inversion, because the
laser transition occurs between a low-lying Stark com- a) b)
–22 2
óESA (10 cm ) 4
F7/2
ponent of the upper and a high-lying Stark component 24 4
H11/2
of the lower laser level [11.836]. During the relaxation 4 4 ô5 = 580 µs
20 I15/2 S3/2 Laser Laser
oscillations at the onset of lasing, a red-shift of the las- 4
I13/2 1.7 µm 850 nm
16 4 4
ing wavelength is often observed in erbium 3 µm laser I11/2 F9/2
12 ESA
systems [11.879–882], because the excitation energy is 4
I9/2
accumulated in the long-lived 4 I13/2 lower laser level and 8
4
the character of the lasing process changes from four- I11/2 ô2 = 6.9 ms
4 Laser
level to three-level lasing [11.836]. For the same reason, 0 2.7 µm
the tunability range of a 3 µm CW laser [11.883] is 780 790 800 810 820 830 840 4
I13/2 ô1 = 9 ms
Wavelength (nm)
narrowed and red-shifted with increasing pump power.
GSA
Pump excited-state absorption (ESA), which is
present in Er3+ at almost all available GSA wave- 4
I15/2
lengths [11.884], has a major influence on the 3+
Er
performance of low-doped, core-pumped erbium 2.7 µm
ZBLAN fiber lasers because of the significant amount Fig. 11.75 (a) Absorption cross sections in ZBLAN:Er3+ near
of ground-state bleaching and excitation of the laser lev- 800 nm: GSA 4 I15/2 → 4 I9/2 and ESA 4 I13/2 → 2 H11/2 , 4 I11/2 →
3/2 , and I11/2 → F5/2 (After [11.874]). (b) Partial energy-
els under these conditions [11.885]. Pumping at 980 nm 4F 4 4

directly into the upper laser level provides the highest level scheme of erbium indicating the processes relevant to the
Stokes efficiency of ηSt = λpump /λlaser = 35% [11.838]. ZBLAN:Er3+ cascade laser: lower loop with GSA to 4 I9/2 , mul-
However, ESA at 980 nm from the 4 I11/2 upper laser tiphonon relaxation, laser transition at 2.7 µm, luminescent decay,
level [11.886] is detrimental to lasing. Experimentally, and upper loop with ESA to 2 H11/2 , thermal relaxation, laser tran-
the best pump wavelength [11.885] is near 792 nm, at the sition at 1.7 µm, multiphonon relaxation, laser transition at 2.7 µm.
peak of ESA from the 4 I13/2 lower laser level [11.874]; Competitive lasing at 850 nm is suppressed in the cascade regime
672 Part C Coherent and Incoherent Light Sources

lasing regime with additional lasing at the transition similarly preventing energy recycling by ETU [11.896].
13/2 → I15/2 near 1.6 µm was demonstrated [11.890].
4I 4 Each pump photon can at best produce one laser pho-
In ZBLAN fibers with higher dopant concentra- ton in the Er3+ ,Pr3+ -codoped system. The theoretical
tions of typically 1–5 mol % (≈ 1.6–8 × 1020 cm−3 ) and limit of the slope efficiency is given by the Stokes
with the double-clad geometry, ESA is much less efficiency, which is 29% under 800 nm pumping. Ex-
important, because the reduced pump intensity with perimentally, a slope efficiency of 17% and an output
low-brightness diode lasers leads to smaller excita- power of 1.7 W were obtained [11.891] (Fig. 11.76b).
Part C 11.2

tion densities. Currently, the most successful approach Other researchers [11.897] reported output powers of
towards a high-power erbium 2.7 µm fiber laser is 660 mW. Since ESA from both laser levels is negligible,
codoping of the fiber with Pr3+ [11.891, 892]. This idea the system can alternatively be pumped near 980 nm,
was reported already in [11.887, 893, 894] and was pro- which provides a Stokes efficiency of 35%. In this way,
posed for the double-clad fiber laser in [11.895]. In the experimental slope efficiency could be increased to
this approach, the Er3+ 2.7 µm transition is operated 25% [11.898]. With improvements in diode-laser tech-
as a simple four-level laser; see the energy-level scheme nology and an optimized fiber design, an output power
in Fig. 11.76a. The 4 I13/2 lower laser level is depopu- of 5.4 W at 2.7 µm with a slope efficiency of 21% could
lated by the energy transfer process ET1 to the Pr3+ recently be demonstrated from an Er3+ ,Pr3+ -codoped
codopant and fast decay to the ground state by mul- ZBLAN fiber laser [11.892, 899].
tiphonon relaxation within Pr3+ . The energy-transfer The first steps toward pulsed output from erbium
process ET2 from the 4 I11/2 upper laser level to the Pr3+ 3 µm ZBLAN lasers [11.882, 900, 901] were unsatisfac-
codopant is weak [11.821]. The strong lifetime quench- tory in terms of output energies and average powers.
ing of the 4 I13/2 lower laser level significantly reduces There have also been attempts to operate the ZBLAN
ground-state bleaching and excitation of the laser lev- fiber laser in the energy-recycling regime. The pa-
els, thus making the influence of ESA negligible, but rameters Wii of both ETU processes in ZBLAN bulk
glasses [11.821] versus Er3+ concentration are shown in
Fig. 11.73b. The criterion for optimization of the slope
a) b)
4 efficiency in (11.90) is maximizing the ratio W11 /W22 .
F7/2 Outputp power (W)
2
H11/2 2
For Er3+ concentrations of > 2–3 mol % at which ETU
4
S3/2 processes become important, this ratio is ≈ 3, see the
1
D2 dashed line in Fig. 11.73b, a more favorable value than
4
F9/2 reported for LiYF4 :Er3+ [11.851]. Energy recycling by
1 ETU at high Er3+ concentrations [11.902] might lead
4
I9/2 ET2 to output powers at 3 µm on the order of 10 W. In early
4 1 attempts, two research groups tried to exploit energy
I11/2 G4
recycling [11.903, 904], however the slope efficiencies
ET1 0 in these experiments did not exceed the slope efficien-
3 0 2 4 6 8 10 12
4 F4 cies obtained in Er3+ ,Pr3+ -codoped fibers pumped at
I13/2 3 Launched pump power (W)
F3
Laser 3 corresponding pump wavelengths [11.891, 892, 898]. In
F2
3
H6 fibers with relatively large core diameters and there-
GSA
3
H5 fore transverse multimode operation, singly Er-doped
4
with concentrations smaller than those required for
3
I15/2 H4 efficient energy recycling, 3 W of output power was
3+ 3+
Er Pr
obtained [11.905]. With further increase of the core
Fig. 11.76 (a) Partial energy-level scheme of erbium indicating the diameter to 90 µm, the highest pulsed output of > 0.5 mJ
processes relevant to the ZBLAN:Er3+ lifetime-quenching laser: could be demonstrated by the same researchers. Re-
GSA at 980 nm to the 4 I11/2 upper laser level (or at 790 nm to the cently, 8 W of output power with a slope efficiency
4I 4 of 24.4% were demonstrated from a highly Er-doped
9/2 pump level and subsequent multiphonon relaxation to I11/2 ),
4
laser transition to the I13/2 lower laser level, and relaxation to (60 000 ppm) ZBLAN fiber when dual-end-pumping the
the ground state via energy transfer ET1 to the Pr3+ codopant. fiber with 25 W of launched pump power at 975 nm.
The energy transfer ET2 from the 4 I11/2 upper laser level to the This result represents the highest output obtained by the
Pr3+ codopant is weak. (b) Output power at 2.7 µm under 792 nm end of 2005 from a fiber laser near 3 µm. Again, the
pumping. (After [11.891]) achieved slope efficiency of 24.4% is very similar to
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 673

that of 25% obtained with the same pump wavelength in phonon energies, which lead to fast multiphonon relax-
a Er3+ ,Pr3+ -codoped fiber [11.898]. Therefore, it must ation of the excitation of the upper laser level. Therefore,
be concluded that efficient energy recycling with cor- many of the laser transitions reported in the literature re-
respondingly improved slope efficiency similar to the quire cooling of the active device. On the other hand, the
result of 50% in a crystalline host material [11.837] is attractiveness of this wavelength range for a number of
still lacking. applications has inspired the search for host materials
with maximum phonon energies below ≈ 300 cm−1 .

Part C 11.2
Dysprosium-doped solid-state lasers at In crystalline hosts, a flashlamp-pumped, cooled
2.3–2.4 µm and 2.9–3.4 µm Er3+ laser at 4.75 µm [11.614], a CW diode-
The search for new mid-infrared laser transitions de- pumped, cooled Er3+ laser at 3.41 µm [11.911], and
pends entirely on the structure of the energy-level a pulsed diode-pumped room-temperature Er3+ laser
diagram of the rare-earth ions. The Dy3+ ion offers at 4.6 µm [11.912] have been operated. A room-
a rather dense energy-level scheme in the infrared spec- temperature BaY2 F8 :Ho3+ laser was operated at
tral region, resulting in a range of absorption peaks, as 3.9 µm [11.913]. Due to its dense energy-level scheme,
well as a four-level laser transition at 2.3–2.4 µm and Dy3+ offers a large range of possible mid-infrared
a phonon-terminated 3 µm laser transition. The transi- transitions. Recently, room-temperature lasing of Dy3+
tion at 2.3–2.4 µm was among the first laser transitions transitions in the low-phonon host materials CaGaS2
reported and the first to be demonstrated in continuous- and KPb2 Cl5 was demonstrated [11.914], in the for-
wave operation [11.609, 610]. Because of the dense mer material even at 4.31 µm. The longest-wavelength
energy-level scheme of Dy3+ , multiphonon relaxation lasers shown to operate in a solid-state mater-
is an issue of concern in this ion, hence low-phonon host ial are room-temperature 5 µm and 7 µm lasers in
materials may improve its laser performance. Recently, LaCl3 :Pr3+ [11.915, 916].
room-temperature laser emission at 2.43 µm was re- The operation of lasers at wavelengths of
ported in the low-phonon host materials CaGa2 S4 :Dy3+ 3.22 µm [11.917] and 3.95 µm [11.918] has been
and KPb2 Cl5 :Dy3+ . At the 3.4 µm transition, room- obtained from Ho3+ -doped ZBLAN fiber and at
temperature laser oscillation from Dy3+ in BaYb2 F8 3.45 µm [11.919] from Er3+ -doped ZBLAN fiber. It
has been reported [11.906]. The 1100 nm output from was, however, necessary to cool the ZBLAN fiber for
a Yb3+ -doped silica fiber laser has been successfully the 3.45 µm and 3.95 µm transitions. These two laser
used to pump a Dy3+ -doped fluoride fiber laser [11.907]. transitions span five or six maximum phonon ener-
In this case, a maximum output power of 275 mW was gies in ZBLAN, therefore the lifetime of the upper
generated with a slope efficiency of only ≈ 5%, however, laser level for each of these transitions is short and en-
when the pump wavelength was increased to ≈ 1.3 µm genders an increase in the pump threshold compared
using a YAG:Nd3+ laser, the slope efficiency is approx- to other ZBLAN fiber lasers operating at the shorter
imately quadrupled to ≈ 20% [11.908]. Reduced levels mid-infrared wavelengths. In addition, the lower laser
of pump ESA are believed to cause this augmentation in levels of these transitions possess quite long lifetimes
the slope efficiency. Future Dy3+ -doped fluoride fiber and some saturation of the output power has been ob-
lasers may benefit from further increases in the pump served [11.920]. This problem (while it can be mitigated
wavelength to 1.7 µm or 2.8 µm. with cascaded lasing), combined with the use of incon-
Before turning our attention to rare-earth-ion-doped venient pump sources has impeded the full utilization
solid-state lasers in the wavelength range beyond 3 µm, of these laser transitions. The 3.95 µm wavelength emit-
it should be noted that solid-state lasers based on the ted from the cooled ZBLAN fiber laser is currently the
actinide ion U3+ have also attracted attention in the longest laser wavelength that has been generated from
recent past [11.909, 910]. a fiber laser.
Generating wavelengths longer than 3 µm from fiber
Solid-state lasers at wavelengths beyond 3 µm lasers is a task that tests the limits of current glass
Laser wavelengths longer than typically 3 µm are gen- technology. The need for lower phonon energies has to
erally difficult to achieve in solid-state host materials be balanced with acceptable mechanical, chemical, and
by direct generation from rare-earth or transition-metal thermal properties. Since the highly developed ZBLAN
ions, because the energy gap between the upper and glass is only useful for laser transitions up to 3–3.5 µm,
lower laser level is necessarily small and all the com- glasses such as the chalcogenides [11.921] will need
mon oxide and fluoride host materials possess maximum to fill the gap. It is because these glasses have to
674 Part C Coherent and Incoherent Light Sources

be drawn into low-loss fiber that has prevented long- sitizer and quenching ions will enable the production of
wavelength emission to the extent that is possible in efficient > 3 µm output some time in the future.
crystalline-based solid-state lasers. Creating efficient,
high-power mid-infrared fiber lasers with output wave- Conclusions
lengths > 3 µm is at the forefront of current fiber-laser In the roughly four decades since the demonstration
research efforts. of the first mid-infrared solid-state lasers, thousands of
As mentioned above, fiber lasers operating on laser scientific papers have been published which have re-
Part C 11.2

transitions that have wavelengths > 3 µm will need to ported on lasing in novel host materials, replacement
use glasses, which have very low phonon energies. While of flashlamps by ion-laser and later diode-laser pump
rare-earth-ion-doped heavy-metal oxides [11.925] have sources, ever-growing output powers, higher efficien-
been studied for 2–3 µm mid-infrared emission; to date, cies, larger tunability ranges, shorter pulse durations
there has been no report of laser action for a fiber laser and the like. A general tendency is that, the shorter
comprised of such a glass. Heavy-metal oxides do not the wavelength, the better the laser performance. When
seem to be suitable for lasers at wavelengths beyond we approach longer wavelengths in the mid-infrared
3 µm, because their maximum phonon energies are com- spectrum, we find that the quality and durability of
parable to fluoride glasses and are too high for laser the required low-phonon-energy host materials decline,
transitions beyond 3 µm. Stokes and slope efficiencies decrease, whereas the ther-
The chalcogenide glasses have been doped with mal problems increase. While many crystalline host
a number of rare-earth ions including Ho3+ [11.924], materials and the corresponding laser techniques have
Tm3+ [11.923], Tb3+ [11.923], Dy3+ [11.922], matured during the 1990s, the fast development of high-
Pr3+ [11.926], and Er3+ [11.927, 928] for studies into power, fundamental-mode fiber lasers, which could be
> 3 µm mid-infrared luminescence (Table 11.21). Fiber- witnessed in the 1 µm spectral range, has now also
laser action has been reported, however, only for an reached the mid-infrared spectral region. However, the
Nd3+ -doped GLS glass operating at a wavelength of assumption that, due to its large surface-to-volume ra-
≈ 1 µm [11.929]. Recent demonstrations of fabricating tio, the fiber geometry might avoid all thermal problems
Bragg gratings [11.930], single-mode fibers [11.931] has been questioned by several recent high-power fiber-
and holey fibers [11.932] with chalcogenide glass high- laser experiments in the near- and mid-infrared spectral
light the utility of this glass for fiber-based applications; region. These phenomena are, in principle, not much
however, the purity and toxicity of the starting materials different from the situation found in crystalline lasers.
and the difficulty of making ultralow-loss fiber currently Nevertheless, there remain distinct differences between
impede the widespread use of chalcogenide glass for these two host categories. When flexibility of the res-
mid-infrared fiber-laser applications. Once these obsta- onator design, short pulses, and high peak powers are
cles have been overcome, future > 3 µm fiber lasers required, crystalline lasers have advantages. On the other
will most likely involve the rare-earth ions Pr3+ , Nd3+ , hand, fiber lasers are preferred when high beam quality
Dy3+ , and Ho3+ doped into chalcogenide glass, because or low pump threshold combined with medium CW out-
most of the important mid-infrared transitions relevant to put power are desired. The low pump threshold of fiber
these ions can be accessed with pump-photon wavenum- lasers is an invaluable advantage when cascade-laser
bers < 10 000 cm−1 . Judicious choice of the overall operation is required to depopulate the long-lived ter-
dopant-ion concentration and the use of particular sen- minating level of one laser transition by a second laser
transition. The comparatively low dopant concentrations
Table 11.21 Examples of luminescent transitions investi- that are useful in fiber lasers due to the long interaction
gated as candidates for mid-infrared lasers in sulfide glasses lengths can minimize energy dissipation by interionic
processes but, equally, limit the exploitation of these pro-
Ion λlaser (µm) Transition Ref. cesses as a tool to optimize the population mechanisms
Dy3+ 13/2 → H15/2
3.2 6H 6 [11.922] of a certain laser system, as has been done successfully
Tm3+ 3.8 3 H →3 H
5 4 [11.923] in several of the mid-infrared crystalline laser systems
Ho3+ 3.9 5 I →5 H
5 6 [11.924] discussed above. Although still a great challenge with re-
spect to fabrication process and durability, low-phonon
Dy3+ 11/2 → H13/2
4.3 6H 6 [11.922]
7 F →7 F
crystalline and fiber host materials have the potential to
Tb3+ 4.8 5 6 [11.923]
5 I →5 I
revolutionize CW mid-infrared lasers in the wavelength
Ho3+ 4.9 4 5 [11.924] range between 3–5 µm.
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 675

11.2.5 Transition-Metal-Ion Lasers 3+


Ti :Al2O3
3+ 3+
Ti :BeAl2O4 Cr :Al2O3
Basics 3+ 3+
Ti :YAlO3 Cr :BeAl2O4
In this chapter an overview of transition-metal-ion lasers 3+
Cr :LiCaAlF6
will be given. The main focus lies on the laser charac- 3+
Cr :Be3Al2(SiO3)6 (emerald)
teristics and results, a more spectroscopically oriented 3+
Cr :LiSrAlF6
overview is given in [11.933]. Transition metals are el- 3+
Cr :La3Ga5SiO14

Part C 11.2
2+
ements of the third, fourth and fifth row of elements V :MgF2
2+
in the periodic table. Laser oscillation has so far only V :CsCaF3

been obtained with ions of the transition metals of the 5+ 5+ 5+


Mn :Sr5(VO4)3F, Mn :Sr3(VO4)2, Mn :Ba5(VO4)2
third row (the Fe row; Ti to Cu). Due to the strong
4+
coupling between the electronic levels of the transition- Cr :Mg2SiO4
4+
metal ion with the surrounding field established by the Cr :Ca2GeO4
4+
Cr :Y3Al5O12
crystalline environment, transition-metal-ion lasers are 4+
Cr :Y3ScxAl5-xO12
usually tunable over a wide spectral range up to sev- 2+
Ni :MgO
eral hundred nanometers. These lasers are of interest for 2+
Ni :Gd3Ga5O13
a wide field of applications, e.g., in scientific research, 2+
Ni :MgF2
in medicine, for measurement and testing techniques, 2+
Co :MgF2
ultrashort-pulse generation, and communication. They
2+
can also be used as coherent light sources for second- Cr :ZnSe
2+
harmonic generation, for optical parametric oscillators, Cr :ZnS
2+
and for sum- and difference-frequency generation. Cr :CdMnTe
2+
The energy-level scheme and thus also the spectro- Cr :CdSe
2+
scopic and laser characteristics of a transition-metal ion Fe :ZnSe

in a crystalline field is strongly dependent on the valence


1000 2000 3000 4000 5000
state of the ion, the number of ligands (i. e., the coor- Wavelength (nm)
dination number) and the strength and symmetry of the
surrounding crystalline field. Therefore it is not possible Fig. 11.77 Overview of tunable solid-state lasers based on transition-
to draw some kind of Dieke diagram for the transition- metal-ion-doped crystals
metal ions, as it is possible for the trivalent rare-earth
ions (see the section on 4f–4f transitions in Sect. 11.2.1). over the near-infrared to the mid-infrared. This overview
The energy-level schemes of the transition-metal ions in includes Ti3+ lasers, especially Ti3+ :Al2 O3 , Cr3+
crystalline hosts are in principle described by the so- lasers, Cr4+ lasers and finally Cr2+ lasers. At the end
called Tanabe–Sugano diagrams [11.934–936]. These of this section, other transition-metal-ion lasers are pre-
diagrams are distinguished by the number of electron sented, including Co2+ and Ni2+ lasers. Finally, some
within the 3d electron shell. In these diagrams the en- general comments about transition-metal-ion lasers will
ergy of a specific level of the transition-metal ion is be given in the last section. In Fig. 11.77 an overview
depicted as a function of the crystal field strength. We of lasers based on 3d↔3d transitions of transition-metal
will not describe the quantum-mechanical background ions is given. It can be seen that almost the whole spectral
to obtain these diagrams, which would be beyond the range between 650 nm and 4500 nm is covered.
frame of this handbook. The reader is referred to the
appropriate literature [11.937–942]. Overview of Transition-Metal-Ion Lasers
In comparison to laser systems based on the 4f↔4f Ti3+ lasers. Ti3+ -doped Al2 O3 (Ti:sapphire) has been
transitions of trivalent rare-earth ions, lasers based on intensively investigated as a tunable laser material since
3d↔3d transitions are in general more affected by the first laser operation was reported [11.943, 944].
a higher probability of excited-state absorption, a higher Efficient laser oscillation was obtained in Al2 O3 in
probability of nonradiative decay, and a higher saturation pulsed [11.943,945,946] and continuous-wave [11.945,
intensity, leading to higher laser thresholds. Often laser 947, 948] operation, for further references see [11.213].
oscillation cannot be obtained at all. In the following sec- The tuning range covers more than 400 nm and spans
tion, the focus is on specific transition-metal-ion lasers, approximately 670–1100 nm [11.949]. It has a rela-
ordered according to their laser wavelength from visible tively high emission cross section of approximately
676 Part C Coherent and Incoherent Light Sources

the tuning range and efficiency of other transition-


Energy
metal-ion-doped lasers. The orbital degeneracy of the
Coordination d levels is removed due to the Jahn–Teller effect, which
octahedral tetrahedral
2 2
yields the large absorption and emission bandwidths.
E T2 The room-temperature absorption and emission spec-
tra are shown in Fig. 11.80. Excited-state absorption
transitions occurs to energy levels correlated to charge
Part C 11.2

transfer and conduction-band levels and between the


two Jahn–Teller-split components of the upper (2 E) d
level. In Ti:sapphire, excited-state absorption was not
2 2 observed in the spectral range of emission [11.952]. In
T2 E
Dq
Table 11.22 the laser-relevant parameters of Ti:sapphire
are listed. Besides the favorable spectroscopic and laser
Fig. 11.78 Basic energy-level schemes of 3d1 ions in octa- characteristic, the Al2 O3 host material offers a variety
hedral and tetrahedral coordination of advantageous properties: a high thermal conductivity,
as well as mechanical and chemical hardness.
4.1 × 10−19 cm2 [11.950] at the maximum of the emis- To date, Ti3+ :Al2 O3 is the most common and com-
sion spectrum. A slope efficiency of 62% has been mercially available tunable solid-state laser. Nowadays,
reported [11.951], which is close to the quantum limit it can be pumped with frequency-doubled Nd lasers
in that experiment of 78% (pump wavelength 589 nm, at wavelengths around 532 nm, thus efficient all-solid-
emission wavelength 750 nm). This indicates the low state laser operation is possible. Formerly, Ar+ -ion laser
intrinsic losses of the system. pumping was applied. In commercial systems, overall
The Ti3+ ion belongs to the 3d1 configuration, efficiencies as high as 30% are obtained.
which is very favorable with respect to laser appli- Besides the broad tuning capability of the
cation because of its simple energy-level scheme (see Ti:sapphire laser, its ability for ultrashort-pulse gen-
Figs. 11.78, 11.79). There are only two 3d1 energy lev- eration and amplification is especially exploited. In
els, which diminishes the possibility of excited-state mode-locked operation, pulses as short as 5 fs [11.953–
absorption of the laser radiation, a process that limits 957] and octave-spanning spectra (e.g., 600 nm to
1200 nm [11.957]) have been obtained.
Energy Laser oscillation with reasonable efficiency has
also been reported for Ti3+ :BeAl2 O4 [11.958–961]
Table 11.22 Overview of Ti3+ :Al2 O3 laser-relevant param-
eters [11.948, 950]
Index of refraction 1.76
Absorption cross section 6.5 × 10−20 cm2 (E  c)
ESA Fluorescence lifetime 3.2 µs
2
nr Fluorescence bandwidth ≈ 200 nm
ÄEJT( E)
GSA 2
(FWHM)
em T2
2 Peak emission wavelength 790 nm
E
Peak stimulated emission 4.1 × 10−19 cm2 (E  c)
2 CT
ÄEJT( T2) cross section
Configurational coordinate Q 2.0 × 10−19 cm2 (E⊥c)
Quantum efficiency ≈ 0.9–1
Fig. 11.79 Schematic diagram of the Jahn–Teller effect
Saturation fluence 0.9 J/cm2
for octahedrally coordinated d1 -systems. 2 E, 2 T2 and CT
Dopant concentration 0.1% (weight)
(charge transfer) are the energy levels, GSA, ESA, and em
Growth Czochralski, heat exchange
are ground-state absorption, excited-state absorption, and
Tm 2050 ◦ C
emission, respectively. nr represents the nonradiative de-
Thermal conductivity 28 W/mK
cay via tunneling between the excited state and the ground
state. ∆E JT is the Jahn–Teller stabilization energy Thermal lens ( dn/ dT ) 12 × 10−19 K−1
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 677

(Table 11.23). However, the efficiency as well as the tun-


ing range is smaller than Ti3+ :Al2 O3 , thus this laser has a) Absorption coefficient (cm–1)
no commercial application. In Y3 Al5 O12 [11.962] and Absorption (arb. units)
YAlO3 [11.963, 964] crystals doped with Ti3+ the ob- T = 4K
served efficiencies are very low (Table 11.23). The main E II c
T = 300 K 1Å
reason for this is excited-state absorption in the spec- E II c
10
tral region of emission and absorption [11.952, 965]. In 1 nm

Part C 11.2
Ti3+ -doped systems nonradiative decay processes due to 595 600 605 610 615
phonon-assisted tunneling between the Jahn–Teller-split ë (nm)
excited and ground states also occur, which prevent effi-
5
cient laser oscillation, e.g., in Ti3+ :Y3 Al5 O12 [11.966,
× 10
967].

Cr3+ lasers.
Basics. The Cr3+ ion is almost always found in oc- 0
200 300 400 500 600
tahedral coordination and its energy-level scheme is ë (nm)
described by the Tanabe–Sugano diagram shown in
b) Fluorescence intensity (arb. units)
Fig. 11.81. In low crystal fields, the first excited state
is the 4 T2 level, whereas in strong crystal fields the Fluorescence intensity
2 E level is the first excited state. This means, that ei- (arb. units)
T = 300 K T = 4K
ther broadband emission (4 T2 → 4 A2 ) or narrow-line 1 nm 1Å
emission (2 E → 4 A2 ) occurs. The absorption spectra
are dominated by quartet–quartet transitions, whereas
the excited-state absorption spectra are dominated ei- 620 625 630 635
ë (nm)
ther by quartet–quartet or doublet–doublet transitions
depending on the total spin of the lowest excited state.

Laser characteristics. The first laser was realized in


1960 with ruby, i. e., Cr3+ -doped Al2 O3 [11.968]. In
ruby – due to the strong crystal field experienced by the
Cr3+ ion – the laser oscillation occurs on the 2 E → 4 A2
transition. Thus, ruby is a three-level laser and not 600 700 800 900 1000
tunable over a wide range. Ruby is still a commer- ë (nm)
cially available pulsed laser system with peak output Fig. 11.80a,b Absorption (a) and emission (b) spectra at room
powers in the MW range used for applications in temperature and at 4 K of Ti:sapphire. (After [11.948])
measurement and pulsed holography. Ruby has remark-
able thermo-mechanical properties which allows high
peak power operation, especially in the Q-switched the ground state. Therefore, a four-level laser system is
regime. In 1976, Morris et al. [11.969] realized with realized. To date, the alexandrite laser has found signifi-
Cr3+ -doped BeAl2 O4 (alexandrite) the first tunable cant commercial applications in industry (e.g., marking,
laser based on the Cr3+ ion. The laser transition is writing and printing), scientific research (e.g., fluores-
4 T → 4 A and terminates in the higher vibronics of cence dynamics, fluorescence imaging, LIDAR), and
2 2

Table 11.23 Overview of other Ti3+ -laser materials


Crystal λlaser Tuning range Slope Mode of Pump source Ref.
(nm) (nm) efficiency (%) operation
BeAl2 O4 810 730–950 15 Pulsed SHG Q-switched Nd:YAG (532 nm) [11.959]
- 753–949 0.013 Pulsed flashlamp (10 µs) [11.961]
Y3 Al5 O12 No details given in the reference [11.962]
YAlO3 615 - 0.3 Pulsed SHG Q-switched Nd:YAlO3 (540 nm) [11.963, 964]
678 Part C Coherent and Incoherent Light Sources

4
more than 30 materials. In Table 11.25 an overview of
E/B T1b (t2 e2) reported laser systems is given [11.103, 977]. In general
80
the tuning ranges for Cr3+ lasers are not as broad as for
Ti3+ :Al2 O3 lasers, however, they exhibit the advantage
2
D
of direct diode-laser pumping around 670 nm, i. e., in
2
the spectral region of the 4 A2 → 4 T2 absorption.
60 A1 (t22e)
For Cr3+ laser systems excited-state absorption
Part C 11.2

4 (ESA) plays a very important role and is the main


T1a (t22e)
reason for the observed large differences in the laser ef-
2 4 ficiencies. Due to its energy-level scheme (Fig. 11.81),
F
40 T2 (t22e)
2
spin-allowed ESA transitions are expected either be-
T2 (t23) tween the quartet states (for low-crystal-field hosts) or
2 between the doublet states (in strong-field hosts). These
D 2
2
H, 2P T1 (t23)
2 2
transitions cover a wide spectral range, due to the strong
G
20 E (t23) electron–phonon coupling. Thus, in general, these ESA
4
P transitions overlap with the absorption and emission
bands. The influence of the ESA is strongly dependent
on the host lattice, i. e., on the crystal field experienced
4
F 0 4
A2 (t23) by the Cr3+ ion. In general, it is observed that crystals
0 1 2 3 4
Dq/B
with a medium crystal field for the Cr3+ ion are favor-
able. Furthermore, in some crystals (e.g., the colquirites,
Fig. 11.81 Tanabe–Sugano diagram for octahedrally coor- alexandrite, emerald etc.) the polarization-dependent se-
dinated 3d3 ions, e.g., Cr3+ with C/B = 5.5. The dashed lection rules can be exploited. Cubic hosts are generally
vertical line marks the border between low and high crystal more strongly affected.
field strength
Summary and perspectives for Cr3+ lasers. Cr3+
medicine (e.g., hair and tattoo removal,). Its advan- lasers are generally interesting for laser applications.
tages are its tunability between 700 nm and 820 nm, the High-efficiency diode-pumped and broadly tunable
high heat conductivity of 23 W/mK, which allows high- continuous-wave and mode-locked laser oscillation have
power pulsed operation, and its high slope efficiency been obtained in a variety of crystals. Some laser sys-
of up to 51% [11.970, 971]. Even broader laser tun- tems are commercially available. However, all of these
ing ranges with similar efficiencies were achieved with crystals have specific drawbacks: they have poor thermal
the Cr3+ -doped colquirite crystals LiCaAlF6 , LiSrAlF6 , mechanical properties, the growing process is difficult
and LiSrGaF6 [11.972] (Table 11.25). However, these or the tuning range is small. Therefore Cr3+ lasers are at
crystals suffer from poor thermo-mechanical properties this time in general not competitive with the Ti3+ :Al2 O3
(Table 11.24), which allow only relatively low pump and laser, which offers a broader tuning range, allows shorter
laser powers. The broad tuning range is exploited for pulses in the mode-locked regime and has better thermo-
mode-locked operation with pulse lengths down to 9 fs mechanical properties. Ti3+ :Al2 O3 cannot be pumped
for Cr3+ :LiCAF [11.973]. The crystals also offer the directly with diode lasers; however, advances in the
possibility of efficient laser-diode pumping with laser frequency-doubling technique of neodymium lasers has
diodes at wavelengths around 670–690 nm. Thus com- led to efficient all-solid-state pump lasers which re-
pact, mode-locked laser systems in the low-power range placed the argon-ion laser as pump. Additionally, pump
are possible [11.974–976]. It is interesting to note that laser diodes in the spectral region between 630 nm and
the highest slope efficiency ever obtained with a Cr3+ - 700 nm with high beam quality and output power are
based laser was achieved with Cr3+ :Be3 Al2 (SiO3 )6 currently not available in a satisfactory manner. Con-
(emerald). Also here, however, the thermo-mechanical cerning the research for new Cr3+ laser systems one has
properties are poor and, furthermore, the emerald crys- to take into account that the Cr3+ ion has already been
tal is very difficult to grow in laser quality. For the investigated in a large number of systems. In princi-
most efficient Cr3+ laser materials the relevant laser and ple, new host materials with the perspective of efficient
materials parameters are listed in Table 11.24. Laser os- laser operation should have a medium crystal field for
cillation with Cr3+ -doped systems has been realized in the Cr3+ ion and polarization-dependent optical prop-
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 679

Table 11.24 Materials, spectroscopic and laser parameters of the most important Cr3+ lasers
LiCaAlF6 LiSrAlF6 Alexandrite Ruby
Structure Trigonal Trigonal Orthorhombic Hexagonal
P3̄1c P3̄1c Pnma R3̄c
Lattice parameters (Å) 5.007 (a) 5.084 (a) 9.404 (a) 4.759 (a)
9.641 (c) 10.21 (c) 5.476 (b) 12.989 (c)

Part C 11.2
4.425 (c)
Typical Cr3+ concentration (cm−3 ) ≈ 1019 – 1020 ≈ 1019 –1020 ≈ 1019 – 1020 ≈ 1.6 × 1019
Growth Czochralski Czochralski Czochralski Czochralski
Tm (◦ C) 810±10 766±10 1870 2050
Density (g/cm3 ) 2.99 3.45 3.69 3.98
Thermal conductivity (W/mK) 4.58 (|| a) 3.0 (|| a) 20 33 (|| a)
5.14 (|| c) 3.3 (|| c) 35 (|| c)
Thermal expansion (10−6 C−1 ) 22 (|| a) 25 (|| a) 6 (|| a) 6.65 (|| a)
3.6 (|| c) -10 (|| c) 6 (|| b) 7.15 (|| c)
7 (|| c)
n 1.390 (a) 1.405 (a) n a = 1.7381 ( 800 nm) 1.763 (o)
1.389 (c) 1.407 (c) n b = 1.7436 ( 800 nm) 1.755 (e)
n c = 1.7361 ( 800 nm)
dn/ dT (10−6 /K) -4.2 (|| a) -2.5 (|| a) 13.6 (o)
-4.6 (|| c) -4 (|| c) 14.7 (e)
σem (10−20 cm2 ) 1.3 (π) 4.8 (π) 0.7 2.5
τem (300 K) (µs) 170 67 260 3000
σem τ(10−24 cm−2 s−1 ) 2.2 3.2 1.8 75
λpeak,em (nm) 763 846 697 694.3
∆λ (nm) ≈ 120 ≈ 200 ≈ 75 -
∆λ/λpeak,em ≈ 0.16 ≈ 0.24 ≈ 0.11 -

erties that could help to avoid or at least significantly 3 T excited state and the 3 A ground state is observed.
2 2
reduce excited-state absorption in the spectral region Referring to the Tanabe–Sugano diagram and the indi-
of the emission. Furthermore, good thermo-mechanical cated area of crystal field values for the Cr4+ ion, one
properties are required. would expect – at least in some materials – narrow-line
emission. However, due to lattice relaxation and crys-
Cr4+ lasers. tal field splitting of the excited state, the 3 T2 or one of
Basics. Cr4+ -doped crystals have been of interest as its crystal field components becomes lower than the 1 E
tunable, room-temperature laser materials since the late level.
1980s. In a variety of materials laser oscillation in The most efficient laser oscillation of Cr4+ -doped
different operation schemes has been achieved, see materials was realized in Mg2 SiO4 and Y3 Al5 O12
Table 11.26 and Table 11.28, where an overview of (YAG). The laser data and main spectroscopic data of
the obtained laser results is given. The energy-level these materials are listed in Table 11.26 and Table 11.27.
scheme of the Cr4+ ion in crystals can be described A variety of further host materials for the Cr4+ ion
with the Tanabe–Sugano diagram shown in Fig. 11.82. were also investigated, but with either low efficiency
The absorption spectra are dominated by the three spin- (Table 11.28) or without realization of laser oscillation.
allowed transitions between the 3 A2 ground state and A detailed overview of Cr4+ -doped systems is given
the 3 T2 (3 F), 3 T1 (3 F), and 3 T1 (3 P) excited states. Usu- in [11.933].
ally, the energy levels are strongly crystal field dependent In all Cr4+ -doped materials investigated thus far,
and split, thus the absorption spectra of different mater- there are two main drawbacks for efficient laser oscil-
ials differ significantly. In all materials investigated thus lation or laser oscillation at all: excited-state absorption
far, broadband emission due to the transition between the and nonradiative decay. Investigation of excited-state
680 Part C Coherent and Incoherent Light Sources

Table 11.25 Free-running laser wavelengths, tuning ranges, laser temperatures, slope efficiencies, operation modes and output
power/output energy of Cr3+ -laser materials. (CW: continuous wave, p: pulsed, SHG: second harmonic, fl: flash lamp, dc: duty
cycle, QS: Q-switched, g-sw: gain-switched, ML: mode locked, * discontinuously)
Host material Wavelength Tuning T (K) η (%) Mode Pout /Eout Ref.
(nm) range (nm)
Be3 Al2 (SiO3 )6 684.8 300 p (SHG QS Nd:YAG) [11.988]
757.4 751–759.2 300 p (fl) 6.8 mJ [11.989]
Part C 11.2

765 728.8–809.0 300 34 CW (Kr+ ) ≈ 330 mW [11.990]


768 720–840 300 64 q-CW (3% DC) 1.6 W [11.991,
992]
LiCaAlF6 780 720–840 52.4 CW (5% DC) Kr+ 850 mW [11.972]
780 720–840 300 52 CW (5% DC) Kr+ [11.993]
780 1.55 p – fl 1.8 J [11.993]
LiSrGaF6 820 - 300 51 CW, Kr+ 1W [11.994]
800–900 300 QS (10 kHz), 12 µJ [11.995]
laser diode [11.996]
BeAl2 O4 679.9 77 [11.997]
680.3 77 p (fl) [11.998,
999]
680.3 700–800 300 p (fl) [11.1000]
750 701–794 300 p (fl) 500 mJ [11.1000,
1001]
765 744–788 300 ≈ 0.7 q-CW (ac Hg-lamp) 6.5 W [11.1002]
745–785 300 2.3 CW 20 W [11.1003]
(DC Hg-,Xe-lamp)
750 700–820 300 p (fl 125 Hz) 150 W [11.1004]
755 300 1.2 CW 60 W [11.1004]
750 300 ML (38 ps) [11.1004]
752–790 300–583 p (fl), temp. tuning [11.1005]
700–820 300–583 [11.970,
971, 997,
1006–
1011]
701–818 300 [11.1000]
744–788 300 [11.1002]
701–818 300 2.5 fl 35 W / 5 J [11.970]
680.4 300 0.15 fl-QS (20 ns) 500 mJ [11.970,
1012]
680.4 300 0.15 fl 400 mJ [11.970]
752 726–802 300 51 CW, Kr+ 600 mW [11.971]
752 700–820 [11.969]
753 300 63.8 dye, 645 nm 150 mW [11.1013]
753 300 laser diode, ≈ 640 nm 25 mW [11.1013]
765 300 28 QS SHG Nd: GVO, 150 mW [11.1014]
671 nm (80 kHz)
LiSrAlF6 825 780–920 300 36 CW, Kr+ 650 mW [11.993,
1015]
865 815–915 300 a-ML (30 ps, 160 fs) 3.5 mW [11.1016]
845 780–1010 300 5 p (fl) 2.7 J [11.1017]
834 300 CW (laser diode) 20 mW [11.1018]
870 858–920 300 laser diode, 4.3 mW [11.1019]
electronically tuned
849 810–860 300 laser diode 43 mW [11.1020]
300 p (fl, 5 Hz) 44 W/ 8.8 J [11.1021]
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 681

Table 11.25 (continued)


Host material Wavelength Tuning T (K) η (%) Mode Pout /Eout Ref.
(nm) range (nm)
ScBO3 843 787–892 300 25 CW (3%), Kr+ 250 mW [11.1022]
300 26 CW (10%), Kr+ 275 mW [11.972]
Gd3 Sc2 Ga3 O12 777 745–805 300 11 CW (1:50 DC) 60 mW [11.1023]
785 742–842 300 28 quasi-CW 200 mW [11.1024–

Part C 11.2
1026]
790 300 1 p (10 µs, dye) 10 µJ [11.1027]
766–820 300 0.06 p – fl 20 mJ [11.1028]
300 0.02 p – fl 10 mJ [11.1029]
0.57 p – fl ≈ 70 mJ [11.1030]
Na3 Ga2 Li3 F12 791 741–841 300 18.4 CW [11.54]
Y3 Sc2 Al3 O12 769 9 q-CW, Kr+ 50 mW [11.1031]
Gd3 Sc2 Al3 O12 780 750–800 300 0.24 p – fl 200 mJ [11.1029]
784 765–801 300 0.12 p – fl 110 mJ [11.1032]
784 300 18.5 CW Kr+ 90 mW [11.1025,
1026,
1033]
780 750–810 300 0.38 p – fl 260 mJ [11.1034]
300 QS (p – fl) 30 mJ [11.1034]
784 735–820 300 19 CW, Kr+ 200 mW [11.1031]
780 750–803 300 0.24 p – fl 206 mJ [11.1031]
SrAlF5 921, 935 852–947 300 3.6 q-CW (DC 3%), Kr+ 35 mW [11.1035]
910 15 q-CW (DC 2%), Kr+ [11.1036]
932 825–1011 [11.1037]
930 825–1010 300 10 Kr+ [11.1038]
KZnF3 810, 826 300 1 p – dye (0.5 µs) [11.1039,
1040]
790–826 775–825 20– 260 0.1 CW, Kr+ [11.1039,
1040]
785–865 300 14 CW, Kr+ 85 mW [11.1041]
785–865 p – ruby [11.1042]
780–845 300 3 CW, Kr+ 55 mW [11.1043]
820 766–865 300 14 [11.1044]
ZnWO4 980–1090 77 13 CW 110 mW [11.1026,
1045]
300 p – dye [11.1045]
La3 Ga5 SiO14 960 862–1107 300 7.6 CW (3% DC) 80 mW [11.1046]
815–1110 300 10 p 10 mJ [11.1047]
968 [11.1048]
Gd3 Ga5 O12 769 - 300 10 quasi-CW [11.1023,
1024,
1026]
La3 Ga5.5 Nb0.5 O14 1040 900–1250 300 5 p 10 mJ [11.1047,
1049]
Y3 Ga5 O12 740 - 5 quasi-CW [11.1023,
1026]
Y3 Sc2 Ga3 O12 750 - 5 quasi-CW [11.1023,
1026]
La3 Lu2 Ga3 O12 830 790–850 3 quasi-CW [11.1024,
1026,
1048]
682 Part C Coherent and Incoherent Light Sources

Table 11.25 (continued)


Host material Wavelength Tuning T (K) η (%) Mode Pout /Eout Ref.
(nm) range (nm)
MgO 830 824–878* 2.3 CW, Ar+ 48 mW [11.1050–
1052]
Al2 (WO4 )3 800 q-CW, Kr+ [11.1053]
BeAl6 O10 820 780–920 300 ≈ 0.03 p – fl 6 mJ [11.1054]
Part C 11.2

834 795–874 300 - p – SHG Nd:YAG [11.1055]


Al2 O3 692.9 (R2) 300 p – fl [11.1056]
693.4 300 p – fl [11.1057]
693.4 77 CW, Hg-lamp 4 mW [11.1058]
77 12 CW, Ar+ 42 mW [11.1059]
694.3 (R1) 300 [11.968,
1060–
1065]
700.9 (N2) 77 [11.1066]
704.1 (N1) 77 [11.1066]
767 300 [11.1067]
Y3 Al5 O12 687.4 not tunable ≈ 77 [11.1068]
LiSr0.8 Ca0.2 AlF6 835 750–950 300 1.25 p – fl 1.2 J [11.1069]
847 783–945 300 CW, Kr+ 300 mW [11.1070]
LiSrCrF6 890 300 33 q-CW, TiSa (DC: 2%) 200 mW [11.1071]
ScBeAlO4 792 740–828 300 31 CW, Kr+ [11.1072]
La3 Ga5 GeO14 880–1220 300 5 p 8 mJ [11.1047,
1073]
Sr3 Ga2 Ge4 O14 895–1150 300 3 p 4 mJ [11.1047,
1073]
Ca3 Ga2 Ge4 O14 870–1210 300 6 p 16 mJ [11.1047,
1049]
La3 Ga5.5 Ta0.5 O14 925–1240 300 5 p 6 mJ [11.1047,
1049]
(Ca, Gd)3 (Ga, Mn, Zr)5 O12 774–814 300 12 p – ruby 170 mJ [11.1074]
≈ 777 300 0.08 p – fl 40 mJ [11.1074]
LaSc3 (BO3 )4 934 300 0.65 q-CW, Kr+ 3 mW [11.1075]
(DC: 10%)
LiInGeO4 1150–1480 300 p (g-sw. Ti:Al2 O3 ) [11.1076]
LiScGeO4 1220–1380 300 p (g-sw. Ti:Al2 O3 ) [11.1076]
Li:Mg2 SiO4 1121 1030–1180 300 p (QS Cr3+ :BeAl2 O4 ) [11.1077]
1120, 1130, 285 1.27 CW (Ar+ ) 5.5 mW [11.1077]
1140

absorption has been performed on garnets [11.978– lence state as Cr3+ . Therefore, there is the tendency
980], forsterite [11.981–984], cunyite [11.985], sili- for incorporation of chromium ions in different valen-
cates [11.982] and Wurtzite-type crystals [11.984, 986, cies in the crystals, especially for materials that do not
987]. The nonradiative decay via multiphonon relaxation exhibit an appropriate tetravalent tetrahedrally coordi-
leads to quantum efficiencies far below 100% at room nated lattice site. This is, e.g., the case for Y3 Al5 O12 ,
temperature; see the overview given in [11.933]. The therefore here additional codoping with divalent cations
preparation of Cr4+ -doped crystals requires for most (Mg, Ca) is necessary. But also in Mg2 SiO4 , Cr3+ is in-
materials special conditions before, during or after the corporated into the Mg lattice. No traces of Cr3+ were
growth process. The Cr4+ ion is not as stable in its va- observed in these materials, which do not exhibit an ap-
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 683

Table 11.26 Overview of laser results obtained with Cr4+ :YAG and Cr4+ :Mg2 SiO4 . (CW: continuous wave, lp: long
pulse pumped, g-sw: gain switched, DP: diode pumped, ML: mode locked, CF: crystalline fiber)
Crystal λlaser (nm) Output ηsl (%) Tuning range Mode of operation Ref.
Y3 Al5 O12 1430 7.5 mJ 22 1350–1530 g-sw (55 ns) [11.1078–1083]
1450 1900 mW 42 1340–1570 CW (T = 3 ◦ C) [11.1081, 1083–1085]
1420 58 mJ 28 1309–1596 lp (200 µs) [11.1082, 1083,

Part C 11.2
1086, 1087]
ML [11.1088, 1089]
1440 20 mW 5 1396–1482 CW-ML (26 ps) [11.1090]
1520 360 mW 8 1510–1530 CW-ML (120 fs) [11.1091]
1510 50 mW <1 1490–1580 CW-ML (70 fs) [11.1092]
1540 - - - CW-ML (53 fs) [11.1093]
1569 30 mW DP-ML (65 fs) [11.1094, 1095]
1450 400 mW Nd − YVO4 , ML (20 fs) [11.1096]
1470 80 mW 5.5 1420–1530 DP [11.1097]
1420 150 mW 1.9 - DP-CF [11.1098]
1440 Intracavity Nd:YAG [11.1099]
Mg2 SiO4 CW [11.1100]
1242 38 - CW (duty cycle 1:15) [11.1101, 1102]
1.1 W 26 - CW [11.1103]
DP [11.1104, 1105]
lp [11.1106]
flashlamp pumped [11.1107]
4.95 mJ - 1206–1250 flashlamp pumped [11.1108]
g-sw [11.1106, 1109–1113]
1235 1170–1370 g-sw [11.1114]
370 mW 13 1173–1338 g-sw (1.5 kHz/10kHz) [11.1115]
ML [11.1116–1122]
300 mW - - ML (25 fs) [11.1122]
1300 Nd:YAG, ML (14 fs) [11.1123]
1260 10 pJ - - DP-ML (1.5 ps) [11.1124]
1260 10 mW 5 1236–1300 CW-DP (T = −10 ◦ C) [11.1104]

propriate lattice site for the Cr3+ ion, e.g., Ca2 GeO4 creased significantly. The reason is mainly excited-state
and Y2 SiO5 . However, the laser results obtained with absorption, but the lower crystal quality and increased
Y3 Al5 O12 and Mg2 SiO4 indicate that the laser efficiency nonradiative rate also contribute [11.1125]. A remark-
is not necessarily affected by the presence of Cr3+ . able characteristic – on first sight – is that the Cr4+ :YAG
laser oscillates polarized parallel to one of its main
Laser characteristics. In Table 11.26 an overview crystallographic axes. The laser output was highest
of the laser results obtained with Cr4+ :YAG and when the pump beam of a Nd:YAG laser operating
Cr4+ :Mg2 SiO4 , the materials in which the most effi- at 1064 nm and propagating along the [001]-axis of
cient laser operation has been obtained, is given. In the Cr4+ :YAG crystal is polarized parallel to one of
YAG, the highest slope efficiency obtained thus far in the crystallographic < 100 >-axes of the Cr4+ :YAG
the continuous-wave regime is 42% [11.1085]. The cor- crystal, and was lowest when its polarization was par-
responding input–output curve is shown in Fig. 11.83a. allel to one of the < 110 >-axes (Fig. 11.83b). The
Attempts to improve the laser efficiency by changing the Cr4+ :YAG laser output is polarized and maintains its
crystals composition, i. e., by substituting Lu for Y on polarization while rotating the pump beam polarization.
the dodecahedral site or Sc for Al on the octahedral site When the pump beam polarization is parallel to one
were not successful [11.1086, 1087]. The efficiency de- of the < 110 >-axes, the Cr4+ :YAG laser polarization
684 Part C Coherent and Incoherent Light Sources

Table 11.27 Parameters of Cr4+ -doped Y3 Al5 O12 and Mg2 SiO4
Y3 Al5 O12 (YAG) Mg2 SiO4 (Forsterite)
Structure Ia3d(O10
h ) Pbnm (D16 2h )
Hardness 8.25–8.5 7
Site symmetry S4 m
Growth Czochralski, divalent codopant required Czochralski
(1930±20) ◦ C (1890±20) ◦ C
Part C 11.2

Tm
Cr4+ concentration ≈ 1017 –1018 cm−3 ≈ 1018 – 1019 cm−3
Thermal conductivity 0.13 W/cmK 0.08 W/cmK
Refractive index (λpeak ) 1.81 1.669 (a)
1.651 (b)
1.636 (c)
dn/ dT (undoped) 7.7–8.2 × 10−6 /K 9.5 × 10−6 /K
Density 4.56 g/cm3 3.22 g/cm3
σabs (1064 nm) ≈ 6.5 × 10−18 cm2 ≈ 5.0 × 10−19 cm2
σem (λpeak ) ≈ 3.3 × 10−19 cm2 ≈ 2.0 × 10−19 cm2
σESA (λpeak ) < 0.3 × 10−19 cm2 < 0.2 × 10−19 cm2
τem (300 K) 4.1 µs 3.0 µs
σem τ 1.35 × 10−24 cm−2 s−1 0.6 × 10−24 cm−2 s−1
Quantum efficiency ≈ 0.2 ≈ 0.16
λpeak,em 1380 nm 1140 nm
∆λ ≈ 300 nm ≈ 250 nm
∆λ/λpeak,em ≈ 0.22 ≈ 0.22

switches [11.1084]. This characteristic can be explained With the Cr4+ :Mg2 SiO4 laser, slope efficiencies
by the crystal structure, the location of the Cr4+ ions of up to 38% [11.1102] and output powers around
and the local symmetry they experience. For details, 1.1 W [11.1103] in continuous-wave operation at room
see [11.1126, 1127]. temperature have been realized (Fig. 11.83c. For crys-

Table 11.28 Overview of other Cr4+ -doped laser materials. (CW: continuous wave, lp: long pulse pumped, g-sw: gain
switched, DP: diode pumped. * laser-active center assigned to Cr3+ in [11.1076], Table 11.24)
Crystal λlaser (nm) Output ηsl (%) Tuning range Mode of operation Ref.
Y3 Scx Al5−x O12 1498 (x = 0.5) 23 mJ 10 1394–1628 lp (100 µs) [11.1087]
(YSAG)
1548 (x = 1.0) 4.5 mJ 3 1464–1604 lp (100 µs) [11.1087]
1584 (x = 1.5) 0.9 mJ 0.5 lp (100 µs) [11.1087]
Lu3 Al5 O12 Not given 50 mW 1.5 - quasi-CW [11.1128, 1129]
Ca2 GeO4 [11.1104, 1130–
1132]
1400 0.4 mJ 6.1 1348–1482 g-sw (T = 0 ◦ C) [11.1130, 1133]
1410 20 mW 8.5 1390–1475 CW-DP (T = −10 ◦ C) [11.1104]
LiScGeO∗4 1300 0.1 mJ 3 1220–1380 g-sw [11.1134]
Y2 SiO5 [11.1135, 1136]
1304 20 mW 0.4 - quasi-CW (1:8) [11.1084, 1137]
1348 0.55 mJ 0.4 - lp (200 µs) [11.1084, 1137]
LiNbGeO5 - - - 1320–1430 g-sw (110 K) [11.1138–1140]
CaGd4 (SiO4 )3 O 1370 37 µJ ≈1 g-sw [11.1141]
SrGd4 (SiO4 )3 O 1440 g-sw [11.1141]
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 685

1
E/B T 2, 1E 3
T1b 1T1 1
T2 3
T1a a) Output power (mW)
50 2500
Output coupler
2000 1%
3 2%
T2
40 3.1 %
1 1500 6.1 %
A2

Part C 11.2
3 °C
1000 ë = 1.45 µm
30

1
G
500
1
20 E 0
1
D 0 1 2 3 4 5 6 7
3
P Absorbed pump power (W)
b) Laser output (arb. units)
10
Cr4+ Mn5+
3
A2
3
F 0
0 2 4
Dq/B

Fig. 11.82 Tanabe–Sugano diagram for tetrahedrally coor-


dinated 3d2 ions. The marked area correspond roughly to
the regions of Dq/B values of Cr4+ and Mn5+ . For sim-
plicity, C/B was set to 5.6, although it differs for different
systems
0
0 45 90 135 180 225 270 315 360
tals from the forsterite group the attempts to obtain better Angle <[010]-axis, pump polarization>
laser results by substituting the constituent ions of the c) Output power (W)
host lattice were also not successful. A variety of crys-
tals were investigated [11.1142–1144] (see the overview 1.2
given in [11.933]) but only for Ca2 GeO4 was laser oscil- T = 6.95 %
1 T = 4.9 %
lation obtained. For Ca2 GeO4 excited-state absorption T = 2.3 %
on the laser wavelength is detrimental [11.985]. 0.8 T = 1.25 %
Laser oscillation was also obtained for Cr4+ - 0.6
doped Y2 SiO5 , LiGeNbO5 , CaGd4 (SiO4 )3 O, and
SrGd4 (SiO4 )3 O. The low efficiencies are probably due 0.4
to excited-state absorption and the high nonradiative
0.2
decay rate.
0
Summary and outlook for Cr4+ lasers. Cr4+ :YAG 1 2 3 4 5 6 7
Absorbed pump power (W)
and Cr4+ :Mg2 SiO4 are efficient and broadly tun-
able laser systems for the infrared spectral range Fig. 11.83 (a) Input–output characteristic of a Cr4+ :YAG-
including the very interesting region for telecom- laser (after [11.1085]), (b) Polarization dependence of
munication applications around 1.3 µm and 1.55 µm. a Cr4+ :YAG laser (after [11.933, 1084]), (c) Input–output
Mode-locked operation with pulse lengths as short characteristic of a Cr4+ :Mg2 SiO4 laser (after [11.1103])
as 20 fs for Cr4+ :YAG [11.1096] and 14 fs for
Cr4+ :Mg2 SiO4 [11.1123] were obtained. Also direct concentration in both materials is rather low, yielding
diode-pumped laser operation was realized, however, a low absorption efficiency of the pump light.
with lower efficiencies [11.1094, 1097]. For both sys- The main obstacle for Cr4+ laser materials is excited-
tems, power handling is a problem and the ion state absorption at the emission wavelength, which
686 Part C Coherent and Incoherent Light Sources

important point concerning Cr4+ laser materials is the


E/B nonradiative decay rate. To decrease this rate, crystals
3 with low-energy phonons and/or small electron–phonon
F Quintet states 1
T1 coupling should be used as host materials, e.g., those
Triplet states
3
H Singlet states in which silicon is substituted by germanium or alu-
20 3
T2
minum is substituted by gallium. However, attempts in
this direction have not been successful thus far.
Part C 11.2

5
T2
3
Cr2+ lasers.
T1 Basics. The energy-level scheme of tetrahedrally co-
ordinated Cr2+ is shown in Fig. 11.84. The Cr2+ ion
10 experiences a low crystal field, e.g., in ZnSe the value of
Dq/B is about 0.9. Thus, the 5 T2 level is the ground state
5
E and the 5 E level is the first excited state, whilst all higher-
1
lying levels are triplet and singlet states. In consequence,
A1
the 5 E → 5 T2 emission is a spin-allowed transition,
while all interionic excited-state transitions are spin-
5 forbidden. Such systems are in general very promising
T2 1
5
D 0 A1 for the realization of efficient tunable laser oscillation,
0 1 2 because even in the case of a spectral overlap between
Dq/B
stimulated emission and excited-state absorption, the
Fig. 11.84 Tanabe–Sugano diagram for tetrahedrally coor- transition probabilities for the latter are expected to be
dinated ions with 3d4 configuration, C/B = 4 about a factor of 10 smaller.
Cr2+ -doped chalcogenide crystals have been shown
is present in practically all crystals. Its influence is to be efficient and broadband tunable solid-state lasers
small in systems with an advantageous energy-level for the infrared spectral range between 2 µm and 3 µm.
scheme and/or a crystal structure that supports strong Pulsed, continuous-wave, mode-locked and diode-
polarization-dependent selection rules. A second but less pumped laser operation have been demonstrated in
recent years. Possible applications of these mid-infrared
lasers include scientific research, remote sensing, trace-
ó (10–19 cm2) gas analysis, medicine, biology, materials processing,
and ultrashort-pulse generation.
8
Materials. The choice of host materials for the Cr2+
laser ion is limited due to special conditions. First, the
materials have to exhibit a tetrahedrally coordinated
4
lattice site. A divalent lattice site is also preferably,
because otherwise a charge-compensation mechanism
would have to be established in the lattice. Furthermore,
0 host crystals with low phonon frequencies have to be
óGSA + óSE– óESA
óSE– óESA chosen in order to decrease the possibility of nonra-
óGSA diative decay via multiphonon relaxation. Chalcogenide
–4 óSE crystals, with their tetrahedrally coordinated divalent
cation lattice sites and with phonon energies lower than
1500 2000 2500 3000 400 cm−1 , are thus very suitable with respect to the
Wavelength (nm)
realization of efficient broadband emission in this mid-
Fig. 11.85 σGSA (dashed line), σSE (dotted line), (σGSA + σSE − infrared spectral range. In Table 11.29 some material
σESA ) (thin solid line), and (σSE − σESA ) spectrum (thick solid line) parameters of the investigated chalcogenide crystals are
of Cr2+ :ZnSe at room temperature. The sharp structure beyond given in comparison to the data for Al2 O3 . The ther-
2500 nm is attributed to the water absorption in air and the following mal conductivities of the chalcogenides are rather high
normalization process. (After [11.1145]) and comparable to the values for Al2 O3 . However, the
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 687

Table 11.29 Materials parameter of some chalcogenide crystals suitable for Cr2+ . The data for Y3 Al5 O12 are given for comparison.
(*: for CdTe). (After [11.1146–1148]) w: Wurtzite, z: Zincblende
ZnS ZnSe Cd1−x Mnx Te CdSe Y3 Al5 O12
Structure Wurtzite: hexagonal Zincblende: cubic Zincblende: cubic Wurtzite: hexagonal Garnet: cubic
Zincblende: cubic
Site symmetry C3v (hex.) Td Td C3v D2 , C3i , S4

Part C 11.2
Td (cubic)
Growth Vertical Brigdeman Vertical Bridgeman Vertical Brigdeman Vapor transport Czochralski
Tm (◦ C) w: 1700 1525 1070–1092 1250– 1350 1930
z: 1020
Hardness (Knoop) w: 210– 240 130 45∗ 70 1250
z: 150– 160
Refractive index 2.29 2.48 2.75 2.57 1.8
Thermal conductivity w: 17 18 ≈2 6.2 10
(W/mK) z: 27 (6.2∗ )
dn/ dT (10−6 /K) w: 46 70 107∗ 9
Transmission range w: 0.4–17 0.5–18 1–28∗ 0.8–18 0.2–10
(µm) z: 0.4–14

main disadvantages of the chalcogenide crystals are the spectrum due to the 5 E → 5 T2 transition is also broad
growth techniques, which are Bridgman or vapor trans- and occurs between 2 µm and 3 µm. The absorption
port, which usually lead to a lower crystal quality than and emission cross sections for the Cr2+ -doped chalco-
in the case of growth by the Czochralski method, and genides are on the order of ≈ 10−18 cm2 ; these are values
the high values for dn/ dt, which lead to strong thermal expected for tetrahedrally coordinated transition-metal
lensing during laser operation, especially in the case of ions and are larger than those for Ti3+ :Al2 O3 [11.948].
high-power operation. The room-temperature absorption and emission spec-
tra are shown in Fig. 11.85. The emission lifetimes at
Spectroscopy. The spectroscopy of Cr2+ ions in chalco- room temperature are on the order of several µs and the
genide crystals has been thoroughly investigated in the emission quantum efficiencies are close to unity. The
past [11.1154–1162]. Tetrahedrally coordinated Cr2+ σem τ product gives an indication of the expected laser
ions exhibit a broad band in the absorption spectrum due threshold, because Pthr ∝ (σem τ)−1 . The values for the
to the 5 T2 → 5 E transition in the infrared spectral range Cr2+ -doped chalcogenides are higher than in the case
with a maximum around 1.7–1.9 µm. The emission of Ti3+ :Al2 O3 , so that generally lower laser thresholds

Table 11.30 Overview about the spectroscopic characteristics of Cr2+ doped chalcogenide crystals. Data for Ti3+ :Al2 O3
are given for comparison
ZnS ZnSe ZnTe Cd0.85 Mn0.15 Te Cd0.55 Mn0.45 Te CdSe Ti3+ : Al2 O3
[11.1149– [11.1149– [11.1149– [11.1152] [11.1153] [11.1154] [11.948]
1151] 1151] 1151]
σabs (10−20 cm2 ) 52 87 123 ≈ 270 ≈ 170 300 6.5
σem (10−20 cm2 ) 75 90 188 270 170 200 45
τem (300 K) (µs) 8 9 3 1.4 4.8 6 3
σem τ 6.0 8.1 5.6 3.8 8.2 12.0 1.4
(10−22 cm−2 s−1 )
η ≈ 0.73 ≈1 ≈1 ≈ 0.38 ≈1 ≈1 ≈ 0.9
λpeak,em (nm) 2300 2300 2400 2250 2480 2200 800
∆λ (nm) ≈ 780 1000 ≈ 900 ≈ 500 770 ≈ 550 300
∆λ/λpeak,em ≈ 0.34 ≈ 0.43 ≈ 0.38 ≈ 0.22 0.31 ≈ 0.25 0.38
688 Part C Coherent and Incoherent Light Sources

for the Cr2+ -doped materials are expected. The ratio be- experiment, a Q-switched Tm,Ho:YLF laser operating
tween the emission bandwidth and the central emission at 2.05 µm with a repetition rate of 10 kHz was used
wavelength, ∆λ/λpeak,em , is a measure for the principle as the pump source. An output power of 4.27 W with
ability to generate ultrashort pulses in the mode-locked a slope efficiency of 47% with respect to the absorbed
regime; the higher this value, the shorter the pulses. The pump power was obtained. The other possibility is to
values for Cr2+ -doped crystals are comparable to those use a rather large pump beam radius of 260 µm (1/ e2
of Ti3+ :Al2 O3 , for which laser pulses shorter than 5 fs radius), as was done by Alford et al. [11.1169]. Using
Part C 11.2

have been realized. However, one has to keep in mind a 35 W Tm3+ :YAlO3 as the pump laser, a continuous-
that bandwidth is not the only important parameter for wave output power of 7 W at 2.51 µm was achieved.
ultrashort-pulse generation. Other important parameters Besides ZnSe, other chalcogenide and mixed chalco-
are the nonlinearities of the material and the thermal genide host materials for the Cr2+ ion are also suitable
lensing introduced by the high peak power, which oc- for efficient laser oscillation. For Cr2+ -doped ZnS, the
curs in the mode-locked regime. Only recently Sorokina spectroscopic characteristics are very similar to those
et al. [11.1163] obtained mode-locking in the fs regime, of Cr2+ :ZnSe. From the material point of view, ZnS
after a lot of work was spent in order to understand even seems to have some advantages over ZnSe as ZnS
the mechanisms behind the pulse-forming processes and has a higher bandgap energy (3.84 eV for ZnS, 2.83 eV
how they can be controlled. In Table 11.30 the main for ZnSe), a higher hardness, a higher thermal con-
spectroscopic data for the Cr2+ -doped chalcogenides are ductivity [27 W/mK for ZnS (cubic phase), 19 W/mK
summarized in comparison to the data for Ti3+ :Al2 O3 . for ZnSe] and a lower dn/ dT (46 × 10−6 1/K for ZnS,
For the tetrahedrally coordinated Cr2+ ion strong 70 × 10−6 1/K for ZnSe) (Table 11.29). However, ZnS
ESA transitions due to inner-shell 3d transitions are is much more difficult to grow and many different
not expected, because all possible transitions are sup- structure types exist. Thus far, the obtained laser re-
posed to be spin-forbidden. This assumption was proven sults for Cr2+ :ZnS are not as good as the results for
by ESA measurements [11.1145, 1164] (Fig. 11.85). Cr2+ :ZnSe (Table 11.31). The highest output power ob-
Neither in the spectral region of the ground-state ab- tained was about 700 mW at an absorbed pump power
sorption nor in the emission region is ESA observed. of 2.65 W from an Er-doped fiber laser [11.1170, 1171].
Tunability up to and beyond 3 µm was predicted for The thresholds are around 100 mW and are thus com-
Cr2+ :ZnSe [11.1145]. This prediction was later proven parable to those observed for Cr2+ :ZnSe. The widest
with laser experiments, where laser oscillation was ob- tuning range obtained so far is 2110–2840 nm. The
served up to 3100 nm [11.1165]. highest slope efficiency in CW regime is about 40%.
Direct diode pumping has also been realized, with an
Laser results. Laser materials based on the Cr2+ ion output power of 25 mW at an absorbed pump power
as the active ion have been investigated since the mid of 570 mW [11.1170]. However, in the same setup
1990s. Nowadays, Cr2+ lasers are operating in a vari- a Cr2+ :ZnSe laser showed better results. Investigations
ety of different operation schemes and under different revealed that the passive losses of the Cr2+ :ZnS crys-
excitation sources. In Table 11.31 an overview of the tal (14%/cm) were much higher than the losses from the
obtained laser results is given. Cr2+ :ZnSe crystal (4%/cm), indicating the larger prob-
The best laser results were thus far obtained for lems with crystal growth and crystal quality in the case
Cr2+ :ZnSe. In different setups using different pump of Cr2+ :ZnS compared to Cr2+ :ZnSe.
sources (Tm3+ lasers, Co2+ :MgF2 lasers, diode lasers Compared to ZnSe and ZnS, the thermal properties
between 1.54 µm and 2.0 µm, erbium-doped fiber am- and material parameters of Cd0.55 Mn0.45 Te are much
plifiers) slope efficiencies up to 73%, output powers up worse, i. e., the dn/ dT is higher and the thermal con-
to 7 W, thresholds lower than 100 mW, a tuning range of ductivity is lower (Table 11.29). Therefore, efficient
2000–3100 nm and mode locking with pulse durations laser operation was only achieved under pulsed pump-
as short as ≈ 100 fs were obtained (Table 11.31). McKay ing [11.1153]. An output power of 170 mW with a slope
and coworkers [11.1166] reported results of a thin-disc efficiency of 64% was realized for a repetition rate of
laser setup for a Cr2+ :ZnSe laser, a setup that was suc- 2 Hz; the tuning range was 2.17–3.01 µm [11.1153].
cessfully applied to Yb-doped laser materials [11.1167]. Mond et al. [11.1172] reported diode-pumped CW op-
This setup appears to be favorable also for Cr2+ :ZnSe, eration with an output power of 6 mW and a slope
because Wagner et al. [11.1168] reported on thermal efficiency of 4%. A thermal rollover at higher pump
rollover in the case of high-power pumping. In McKay’s powers was observed, indicating the strong thermal lens-
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 689

Table 11.31 Overview of the laser results obtained for Cr2+ -doped materials
ZnS ZnSe Cd0.85 Mn0.15 Te Cd0.55 Mn0.45 Te CdSe CdTe
λlaser (nm) 2350 [11.1149, 1173] 2350 [11.1149] 2515 nm [11.1152] 2550 [11.1153] 2600 [11.1174] 2535
2500 [11.1145] 2660 nm [11.1175] [11.1176]
2600 [11.1164]
3000 [11.1164]

Part C 11.2
ηsl (%) 40 [11.1170] 73 [11.1145] 44 [11.1175] 64 [11.1153] 50 [11.1177] 1 [11.1176]
Tuning (nm) 2050–2400 2000–3100 2300– 2600 2170–3010 2400–3400
[11.1178] [11.1165] [11.1175] [11.1153] [11.1179]
2110–2840
[11.1170]
Pout or E out 0.1 mJ 7W 0.6 mJ 170 mW (2 Hz) 0.5 mJ pulsed
[11.1149, 1173] [11.1169] [11.1175] [11.1153] mode
Pulse length (ML) 4.4 ps [11.1180,
1181]
≈ 4 ps [11.1182]
≈ 100 fs
[11.1163]
Other references
Pulsed [11.1149–1151, [11.1149–1151, [11.1152, 1175, 1183] [11.1153, 1183] [11.1174, 1177,
1170, 1171, 1173, 1173] 1179, 1184]
1178]
CW [11.1145, 1164,
1168, 1185–
1189]
Gain-switched [11.1190]
Diode pumped [11.1145, 1165,
1172, 1191–
1198]
Mode-locked [11.1180, 1182]
Thin disc [11.1166]
Multi-wavelength [11.1199]

ing problems. The threshold pump power was only was 815 mW [11.1184] while the largest tuning range
120 mW. This low value is expected from the spec- achieved thus far is 2.4–3.4 µm [11.1179].
troscopic parameters. Under diode pumping at a duty
cycle of 1:4, the thermal rollover is not observed at the Outlook for Cr2+ systems. Cr2+ -doped materials are
pump powers available. Then the highest output power highly efficient lasers in a very interesting wavelength
is 15 mW with a slope efficiency of 5% and a threshold range for application; see the overview in Table 11.31.
of ≈ 100 mW. In all materials investigated, the material parameters are
Cr2+ :CdSe exhibits a similar behavior to still a large problem, i. e., the quality of the crystals, the
2+
Cr :Cd0.55 Mn0.45 Te, as expected from the material strong thermal lensing, the high nonlinearity, yielding
parameters and spectroscopic characteristics. Thus also a strong tendency for self-focusing, and the relatively
strong thermal lensing and power-handling problems are low damage threshold. All these problems are most se-
encountered in the laser experiments. CW laser opera- vere for CdMnTe and CdSe. Therefore, the thin-disc
tion has not yet been reported, however, the laser results setup may be a way to overcome some of these prob-
under pulsed pumping are very promising. Using a Q- lems. Another alternative is the use of larger pump and
switched Tm,Ho:YAG laser operating at 2.05 µm with laser modes. As far as ultrashort-pulse generation is con-
a repetition rate of 1 kHz, a maximum output energy cerned, Sorokina et al. recently realized mode locking in
of 0.5 mJ per pulse and a slope efficiency of 50% was the fs regime [11.1163]. Thus far, only a few materials
obtained [11.1177]. The highest average output power have been investigated for laser applications. Therefore,
690 Part C Coherent and Incoherent Light Sources

there is the possibility to look for different host materials 1


for the tetrahedral Cr2+ ion, e.g., ZnGa2 S4 , ZnGa2 Se4 , E/B T 2, 1E 3
T1b 1T1 1
T2 3
T1a
50
CaGa2 S4 , and CaGa2 Se4 .

Other transition-metal-ion lasers. 3


T2
V2+ lasers. The V2+ ion is isoelectronic to the Cr3+ 40
1
ion. Therefore, its energy-level scheme can also be A2
Part C 11.2

described with the Tanabe–Sugano diagram shown in


Fig. 11.81. The absorption spectra of octahedrally coor- 30
dinated V2+ is similar to that of Cr3+ , but red-shifted
due to the lower valence of the V2+ ion. The spectra 1
G
are dominated by the three broad spin-allowed bands 1
20 E
due to transitions between the 4 A2 (4 F) ground state 1
D
and the 4 T2 (4 F), 4 T1 (4 F), and 4 T1 (4 P) excited states. 3
P
The emission spectra consist of a broad band due to
the 4 T2 (4 F) → 4 A2 (4 F) transition, also shifted to longer 10
wavelengths compared to the emission spectra of Cr3+ .
Laser oscillation with V2+ on the 4 T2 (4 F) → 4 A2 (4 F) Ni2+ 3
A2
transition was realized only in MgF2 [11.1200–1202] 3
F 0
0 2 4
and CsCaF3 [11.1203, 1204]. An overview of the ob- Dq/B
tained laser results is given in Table 11.31. The laser
efficiencies are very low. Payne et al. [11.44, 1205] and Fig. 11.86 Tanabe–Sugano diagram for the d8 electron con-
Moncorgé et al. [11.1206] found that ESA is the domi- figuration. The dashed area corresponds to the Dq/B values
nant loss mechanism for laser oscillation. In some mater- of Ni2+
ials nonradiative decay also competes with the emission,
leading to small emission quantum efficiencies. measurements of the ESA for several Ni2+ -doped crys-
tals were performed by Koetke et al. [11.1207, 1208].
Ni2+ lasers. The energy-level scheme of octahedrally With increasing temperature the excited-state absorp-
coordinated Ni2+ in crystals can be described with the tion and ground-state absorption bands become broader
Tanabe–Sugano diagram shown in Fig. 11.86. In the and thus overlap to a larger extent with the stimu-
absorption spectra, three bands according to the spin- lated emission. As a result, the spectral region where
allowed transitions from the 3 A2 (3 F) ground state to the σeff = σse − σESA > 0 becomes narrower. Furthermore,
3 T (3 F), 3 T (3 F), and 3 T (3 P) excited states are ob- the losses due to ground-state absorption increase. How-
2 1a 1b
served. The laser transition of Ni2+ lies in the infrared ever, at low temperatures output powers up to 10 W and
spectral range due to the 3 T2 (3 F) → 3 A2 (3 F) transition. slope efficiencies up to 57% were obtained [11.1202].
Its spectral position is strongly wavelength dependent
(Table 11.33). The emission lifetime is typically on the Mn5+ lasers. The Mn5+ ion incorporates into crys-
order of ms and the emission quantum efficiency is near tals mainly at tetrahedrally coordinated lattice sites. Its
unity at room temperature in most materials. energy-level scheme can be described with the Tanabe–
Despite these advantageous spectroscopic data, laser Sugano diagram shown in Fig. 11.82. Compared to Cr4+ ,
oscillation with Ni2+ was obtained only at temperatures the crystal field is higher due to the higher valence
below 240 K and only in a few materials (Table 11.33). state, thus the Mn5+ ion exhibits narrow-line emis-
The absence of laser oscillation at room temperature can sion due to the 1 E(1 D) → 3 A2 (3 F) transition. Optical
be explained by excited-state absorption (ESA), which properties of Mn5+ ions in solids have been under
overlaps with the spectral range of emission. Detailed investigation for more than 30 years [11.1209–1217].

Table 11.32 Overview of V2+ -laser materials


Host material λlaser (nm) Tuning range (nm) T (K) Mode of operation Pout /Eout η (%) Ref.
MgF2 1121 1070–1150 77 pulsed [11.1200–1202]
CsCaF3 1280 1240–1330 80 CW ≈ 15 µW 0.06 [11.1203, 1204]
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 691

Table 11.33 Overview of the results of Ni2+ lasers


Host material λlaser (nm) Tuning range T (K) Mode of operation Pout /Eout η (%) Ref.
(nm)
MgO 1314.4 77 Pulsed [11.1200]
1318 80 CW 10 W 57 [11.1202,
1223]
≈ 1320 [11.1202]

Part C 11.2
≈ 1410 [11.1202]
MgF2 1610–1740 89 CW, CW-Q-qw 1.85 W 28 [11.1202]
1608–1730 80 CW 185 mW 10 [11.1224]
1610–1740 80 CW ≈ 100 mW [11.1225,
1226]
1670 80 QS (480 ns) 25 mW (1 kHz) [11.1225]
1610–1730 ML (23 ps) ≈ 100 mW [11.1227]
1623 77 Pulsed [11.1200,
1228, 1229]
1630 20–90 CW 1.74 W 37 [11.1230]
1730–1750 100–200 CW ≈ 0.5 W [11.1230]
1636 77–82 Pulsed [11.1200]
1674–1676 82–100 Pulsed, CW [11.1200]
1731–1756 100–192 Pulsed, CW [11.1200]
1785–1797 198–240 Pulsed [11.1200]
MnF2 1865 20 Pulsed [11.1200]
1915 77 Pulsed [11.1200]
1922 77 Pulsed [11.1200]
1929 85 CW (exc.) [11.1200]
1939 85 CW (exc.) [11.1200]
KMgF3 1591 77 Pulsed [11.1231]
CaY2 Mg2 Ge3 O12 1460 80 Pulsed ≈ 3.8 mJ 0.7 [11.1202,
1229]
Gd3 Ga5 O12 1434–1520 100 Pulsed 6 [11.1207,
1232]

Mn5+ laser operation at room temperature was demon- energy level. However, thus far Mn5+ systems exhibiting
strated by Merkle et al. in Ba3 (VO4 )2 , Sr3 (VO4 )2 , broadband emission are not known.
and in Sr5 (VO4 )3 F [11.1218–1220]. The laser tran-
sition is realized between the 1 E(1 D) excited state Co2+ lasers. The Co2+ ion in octahedral coordination ex-
and the 3 A2 (3 F) ground state, thus these lasers are hibits laser oscillation in the mid-infrared spectral region
three-level systems. The efficiency is rather low (laser between 1.5 µm and 2.5 µm. Its energy-level scheme
output energy ∼ µJ, ηsl ≤ 1.6%) and laser oscillation can be described with the Tanabe–Sugano diagram for
from other Mn5+ systems has not been reported. The the 3d7 electron configuration shown in Fig. 11.87.
major drawback for these lasers is the excited-state Three broad and spin-allowed transitions between the
absorption at the stimulated-emission wavelength. In- 4T 4 4 4
1a ground state and the T2 , A2 and T1b ex-
vestigations of the excited-state absorption and gain cited states exist. In MgF2 , these transitions are located
were performed in detail by Verdún [11.1217], Merkle around 7000 cm−1 , 15 000 cm−1 , and 20 000 cm−1 , re-
et al. [11.1218], Manaa et al. [11.1221] and Kück spectively [11.1233]. The emission occurs between
et al. [11.933, 1222]. 1.5 µm and 2.5 µm, according to the 4 T2 → 4 T1a transi-
To obtain a four-level system, one should search tion. At low temperatures, the lifetimes are on the order
for crystals with low crystal field strengths or with of several ms, while at room temperature the emis-
large energy-level splittings. Then the 3 T2 (3 F) or one sion is strongly quenched due to nonradiative decay
of its crystal field components would be the lowest- via multiphonon relaxation, yielding very low quantum
692 Part C Coherent and Incoherent Light Sources

Co2+ :MgF2 , which is also a commercial laser system.


E/B 2
A2 4A2 2
A1
4
T1
With Co2+ :MgF2 an overall tuning range of 1.5–2.5 µm
70
was realized with output powers up to 4.2 W, output
energies up to 1.6 J and slope efficiencies as high as
4 65%. As the pump source, Nd:YAG or Nd:glass lasers
T2
around 1.3 µm are usually used, however, laser oscilla-
50 tion has also been realized under flashlamp pumping,
Part C 11.2

argon-ion laser excitation and oxygen–iodine laser exci-


2
tation. Operation regimes are CW, pulsed, Q-switched
2 T2
F 2
T1
and mode-locked.

30 Fe2+ lasers. The Fe2+ ion has a 3d6 electron configu-


ration that is complementary to that of Cr2+ . The 5 D
4
T1
free-ion state also splits into a 5 T2 and a 5 E state,
2
G however, for the Fe2+ ion 5 E is the ground state and
4
P 5 T is the first excited state. Consequently, there is just
4
T2 2
10
2 one spin-allowed absorption (5 E → 5 T2 ) and emission
E
4
T1
(5 T2 → 5 E) transition. As for the Cr2+ ion, all excited-
4 2
F 0 E state transitions are spin-forbidden. Thus, one might
0 1 2 3 4
Dq/B
expect similar laser characteristics for Fe2+ -doped lasers
as for Cr2+ lasers. However, the energy gap between the
5 T excited state and the 5 E ground state is smaller, thus
Fig. 11.87 Tanabe–Sugano diagram for the d7 configuration 2
(after [11.36]) the emission is at longer wavelengths and the nonradia-
tive decay rate is higher, leading to lifetime shortening
efficiencies [11.1234]. Excited-state absorption over- and low quantum efficiencies at elevated temperatures.
laps with the 4 T1a → 4 T2 absorption band, which is For Fe2+ :ZnSe, the emission lifetime first increases from
the main pump band for laser operation. In the region 12 to 120 K from 33 µs to 105 µs and then decreases to
of stimulated emission, the excited-state absorption is about 5 µs at 250 K due to thermally activated multi-
negligible [11.1233]. phonon decay [11.1235, 1236]. At 14 K, the 5 E → 5 T2
Laser oscillation was obtained in the continuous- absorption band is between 2.5 µm and 3.75 µm, and the
wave regime only at cryogenic temperatures, while 5 T → 5 E emission band is between 3.7 µm and 4.8 µm.
2
pulsed laser operation was also realized at room temper- Laser oscillation of Fe2+ was obtained in
ature for Co2+ -doped MgF2 and KZnF3 . An overview ZnSe [11.1235–1239] and in n-InP [11.1240]. For
of the laser results for Co2+ laser systems is given in Fe2+ :ZnSe, room-temperature tunable laser oscil-
Table 11.35. The best laser results were obtained for lation was recently reported in a gain-switched
Table 11.34 Overview of Mn5+ -laser materials. The data are from the literature stated in the text [11.1209, 1222]
Ba3 (VO4 )2 Sr3 (VO4 )2 Sr5 (VO4 )3 F
Structure Hexagonal, R-3m Hexagonal, R-3m Hexagonal, P63 /m
Site symmetry C3v (V-site) C3v (V-site) Cs (V-site)
Growth Czochralski/LHPG Czochralski/LHPG Czochralski
Tm (◦ C) 1560 1923
σabs (10−20 cm2 ) ≈ 300 ( 800 nm) ≈ 300 ( 800 nm)
σem (10−20 cm2 ) 10–20 27 (E  c), 13 (E⊥c)
σESA (10−20 cm2 ) 14 (E  c), 24 (E⊥c)
τem (300 K) (µs) 430–480 525 475–500
σem τ (10−22 cm−2 s−1 ) ≈ 0.7 ≈ 1.3 (E  c), ≈ 0.6 (E⊥c)
λlaser (nm) 1181.0 1168.0 1163.7
ηsl (%) 0.21 0.08 1.6
Pout or E out ≈ 2 µJ ≈ 1 µJ
Lasers and Coherent Light Sources 11.2 Solid-State Lasers 693

Table 11.35 Overview of Co2+ -laser materials. (*: versus input power, QS: Q-switched operation, ML: mode-locked
operation)
Host material λlaser (nm) λlaser (nm) T (K) Mode of operation Pout /Eout η (%) Ref.
MgF2 1860 1500–2000 80 CW 1W 31 [11.1241]
1920 1600–2300 80 Pulsed 150 mJ 65 [11.1202, 1242,
1243]
1920 80 Pulsed 7.3 W (50 Hz) ≈ 23∗ [11.1242,1243]

Part C 11.2
1920 QS (220 ns) 25 mJ [11.1242,1243]
1940 225 Pulsed ≈ 11 mJ 14∗ [11.1243]
1920 80 4.2 W 28∗ [11.1202,1243]
2100 1750–2500 RT Pulsed 70 mJ 46 [11.1244]
1650–2010 80 ML (34 ps) [11.1227]
1500–2000 QS-ML (200 ps) 400 mW (ave) [11.1245]
1600–1900 77 QS (600 ns) 15 mJ [11.1246]
1890 1600–2150 77 CW 2W 32 [11.1247]
2050 RT Pulsed 0.2 mJ 29 [11.1248]
2050 77 Pulsed 1.6 J 44 [11.1249]
2040 1960–2180 RT Pulsed 20 mJ 25 [11.1233]
1630–2080 80 CW ≈ 100 mW 5 [11.1226,1250]
1750 77 Pulsed [11.1200,1251]
2060 1800–2450 282 Pulsed 900 mJ 33∗ [11.1252]
1803.5 77 Pulsed [11.1200,1251]
1990 77 Pulsed [11.1200,1251]
2050 77 Pulsed [11.1200,1251]

KMgF3 1620–1900 80 CW 20 [11.1253]


1821 77 Pulsed [11.1200]
KZnF3 1650–2110 80 30 [11.1253]
1770 1650–2070 80 120 mW [11.1254]
1950 1850–2050 85 CW ≈ 20 mW ≈2 [11.1255]
1700–2150 98 CW ≈ 55 mW 8 [11.1256]
2024 300 Pulsed 3 mJ 8 [11.1233]
ZnF2 2165 77 Pulsed [11.1200,1251]

mode [11.1237]. The pump source was the second It was shown that they are efficient (usually tunable)
Stokes output of a Nd:YAG laser at 2.92 µm. The out- laser sources covering a wide spectral range (Fig. 11.77).
put pulse energy was about 1 µJ. The highest output However, compared to lasers based on 4fn →4fn transi-
power and slope efficiency of 12 µJ and 8.2%, respec- tions of trivalent rare-earth ions, they play only a small
tively, were obtained at lower temperatures. In this case, role as far as commercialization is concerned. In prin-
the Fe2+ :ZnSe laser was pumped by a pulsed Er3+ :YAG ciple only the Ti3+ :Al2 O3 and – with limitations – the
laser operating at 2.698 µm [11.1235, 1236]. The laser Cr3+ :BeAl2 O4 laser can be mentioned. These lasers are
wavelength is tunable with temperature from 3.98 µm at mainly used in the field of scientific research. The main
15 K to 4.54 µm at 180 K. In n-InP, Fe2+ laser oscillation reason for this is that their advantages, i. e., their tunabil-
was obtained at 2 K at 3.53 µm, i. e., at the zero-phonon ity and their capability to generate ultrashort pulses, are
transition [11.1240]. not relevant for most industrial applications. They ex-
hibit lower output power than lasers based on 4fn →4fn
Summary transitions of trivalent rare-earth ions (e.g., Nd3+ :YAG,
In this chapter an overview of transition-metal-ion- Yb3+ :YAG) and are more expensive and less efficient
doped crystals as solid-state laser materials is given. than diode lasers. Direct diode-laser pumping is either
694 Part C Coherent and Incoherent Light Sources

Table 11.36 Overview about transition-metal ions sorted according to the corresponding Tanabe–Sugano diagram dn
(TSD-dn ). Normal: octahedral coordination; italic: tetrahedral coordination. Light brown: laser oscillation in octahedral
coordination; Dark brown: laser oscillation in tetrahedral coordination. (After [11.933])
Ion TSD-d1 TSD-d2 TSD-d3 TSD-d4 TSD-d5 TSD-d6 TSD-d7 TSD-d8 TSD-d9
Ti Ti3+ Ti2+
V V4+ V3+ V2+ V3+ V4+
Part C 11.2

Cr Cr4+ Cr3+ Cr2+ Cr2+ Cr4+ Cr5+


Mn Mn5+ Mn4+ Mn3+ Mn2+ , Mn2+ Mn3+ Mn5+ Mn6+
Fe Fe2+ Fe3+ , Fe3+ Fe2+ Fe6+
Co Co3+ Co2+ Co3+ Co2+
Ni Ni2+ Ni3+ Ni3+ Ni2+
Cu Cu2+ Cu3+ Cu2+

inefficient or – in the case of Cr3+ and Cr2+ lasers in the pump channel, which also affects the overall
– requires laser diodes that are not yet available at laser characteristics. Thus, its general influence depends
a satisfactory price and quality on the market. strongly on the material parameters of the laser sys-
Transition-metal-ion and especially tunable laser tem, i. e., mainly of the host material. Materials with
systems exhibit a stronger coupling of the electronic a high thermal conductivity and mechanical strength are
levels to the vibrating lattice of the crystal. This leads to favored. As an example, Cr4+ :Y3 Al5 O12 can be given.
higher possibilities for ESA and nonradiative decay pro- Here, the quantum efficiency is less than 20%, whereas
cesses compared to the 4fn →4fn transitions of trivalent laser operation with a slope efficiency close to 40% was
rare-earth ions in crystals. realized.
The main problem in realizing efficient laser oscilla- Table 11.36 gives an overview of the transition-
tion is the excited-state absorption from the metastable metal ions in octahedral and tetrahedral coordination
upper laser level. From (11.87) and (11.88) its ef- investigated to date. They are listed according to
fect on laser threshold and slope efficiency becomes their corresponding energy-level diagram (i. e., Tanabe–
clear. It occurs in principle for every electron configura- Sugano diagram). The laser-active transition-metal ions
tion, either as intra- or interconfigurational transitions are indicated. Almost all transition-metal ions with dif-
or as a transition to charge transfer or conduction- ferent valence states and ligand coordinations have been
band-related levels. The electron configurations are in investigated thus far. Efficient room-temperature laser
general favorable, when intraconfigurational excited- oscillation was only obtained for Ti3+ and Cr3+ in
state absorption transitions are not possible, e.g., in octahedral and for Cr2+ and Cr4+ in tetrahedral co-
the d1 and d9 configuration, or are less strong due to ordination. Whether efficient laser operation will also
selection rules, e.g., in the d4 and d6 configurations. be obtained for other ions depends very much on the
Other configurations exhibit more-complex energy-level host material chosen. For example, the Ti3+ ion ex-
schemes, therefore intraconfigurational ESA transitions hibits efficient laser operation only in Al2 O3 . Therefore,
occur with high probability in the spectral regions of other ions cannot a priori be excluded as efficient laser
emission and excitation. The influence of ESA, how- ions.
ever, can even in this case be reduced, e.g., by taking
advantage of polarization-dependent transition rules, 11.2.6 Overview of the most Important
which result in higher stimulated-emission cross sec- Laser Ions in Solid-State Lasers
tions than ESA cross sections, as it is the case, e.g., for
Cr3+ :LiSrAlF6 and Cr4+ :Y3 Al5 O12 . Research on laser materials has created a number of
The role of nonradiative decay for the realization compact, efficient solid-state laser sources for a large
of efficient laser operation is less important, although variety of applications. Laser materials have been de-
not negligible. It affects to a first approximation only veloped for various wavelengths (near-infrared, visible,
the laser threshold, which is increased (11.84). How- UV) and power regimes (mW to multi-kW). Spe-
ever, a nonradiative rate leads to a temperature increase cial geometries of the active material (microchip, rod,
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 695

disc, fiber) strongly correlate with the active ion con- Near-IR rare-earth lasers.
centrations and cross sections of absorption and gain Nd3+ 0.9, 1.06, 1.3 µm
transitions. Yb3+ 1–1.1 µm
The values of the cross sections depend on the quan- Tm3+ 2 µm, 1.5 µm (upconversion)
tum numbers of the final and initial states as well as on Ho3+ 2 µm
the local environment of the active-ion site in the mater- Er3+ 1.6, 3 µm, 0.85 µm (upconversion)
ial. The lifetimes of the states are influenced by radiative

Part C 11.3
and nonradiative transitions. So, the microscopic crystal Visible rare-earth lasers.
properties play an important role for static and dynamic
processes in the laser crystal. Pr3+ 0.64 µm (diode-pumped)
In the near-infrared spectral region high efficien- Pr3+ ,Yb3+ 0.52, 0.63 µm (upconversion)
cies have been achieved with diode-pumped oxide- Er3+ 0.55 µm (upconversion)
and fluoride-based laser materials doped with the rare- Tm3+ 0.45, 0.48, 0.51, 0.65, 0.79 µm (up-
earth ions Nd3+ , Tm3+ , Ho3+ , Er3+ , and Yb3+ . For conversion)
high-average-power operation Nd3+ - and Yb3+ -doped
crystals are of greatest interest. Especially the Yb3+ Frequency doubling of near IR rare-earth lasers (Nd, Yb)
ion exhibits very small Stokes losses and minimum heat
generation, which reduces thermal lensing and improves UV rare-earth lasers.
beam quality. Transition-metal-doped crystals based on Ce3+ 0.3 µm
the ions Ti3+ , Cr2+ , Cr3+ , and Cr4+ offer broadly tun-
able radiation within the spectral region 680–3000 nm. Frequency doubling of visible rare-earth lasers
In the visible region Er3+ -, Tm3+ -, and Pr3+ -doped Frequency tripling/quadrupling of near-IR lasers
laser materials operate at several red, green, and blue
transitions with laser diode upconversion and/or direct Transition-metal lasers.
pumping. So far Ce3+ is the only ion with reasonable Ti3+ 0.68–1.1 µm
direct laser performance in the UV. Cr3+ 0.7–1.1 µm
The following wavelength data provide a rough Cr4+ 1.2–1.6 µm
guide to the spectral range of the various laser ions. Cr2+ 2–3 µm

11.3 Semiconductor Lasers


11.3.1 Overview a much higher density of electrons than holes and in the
VB close to E V a much higher density of holes than elec-
In crystalline solids the interaction between atomic trons. This extremely nonthermal condition is generated
energy levels generates energy bands. A quantum- by strong electrical or optical pumping of the laser-active
mechanical treatment provides, in the single-electron material. The electrical carrier injection in most cases is
approximation, energy bands which overlap which each obtained by a p–i–n heterojunction made of III/V semi-
other or are separated by bandgaps from each other. conductor materials. Choosing InP as a typical example,
In semiconductors, we find between the energetically Fig. 11.88 displays a planarization (projection into 2-
highest band, which is fully occupied by electrons at D space for simplification) of the real 3-D zinkblende
T = 0 K, the valence band (VB), and the energetically crystal structure with the corresponding band structures
lowest band, which is completely empty at T = 0 K the below. From the left to the right p-InP, intrinsic i-InP
conduction band (CB) an energy range, in which we and p-InP are shown.
find no allowed energy states, disregarding energy states In the highly p-doped InP bulk regions, at room tem-
originating from dopants. This bandgap, E g , is the en- perature nearly all acceptors have released their holes
ergy difference between the lower conduction-band edge into the valence band. Well away from the pn junc-
E C and the upper valence-band edge E V . For laser op- tion the hole field current (drift current) dominates the
eration an extreme deviation from thermal equilibrium carrier transport. At the left edge of the device, holes
(nonthermal carrier distribution) is required: carrier in- are generated under the p contact. At the right edge of
version. In the CB close to E C carrier inversion means the device, electrons are injected through the n contact.
696 Part C Coherent and Incoherent Light Sources

p-doped i = intrinsic, undoped n-doped


a) c) e)

In P In P In P In P In P In P

P Be P In P In P In P In S In
Part C 11.3

In P In P In P In P In P In P

b) E d) E f) E

Extrinsic

EC EC EC

EV EV EV

Extrinsic

y Space y y

Fig. 11.88a–f Schematic of a planarized lattice structure of p-doped, undoped and n-doped InP (a,c,e). Below are the
corresponding band structures in space (b,d,f). The dopants are indicated by squares, the full lines indicate the movement
of electrons, the broken line the movement of defect electrons (=holes) in space and the dotted line the movement of holes
on the VB

Well away from the pn junction the electron field cur- electrically confines electrons in the CB and holes in
rent dominates the carrier transport there. The bandgap the VB, which is visualized by the band edge. Since
E g nearly equals the energy of the photons generated in for semiconductors decreasing E g in nearly all cases
the central intrinsic region. However, such a homojunc- increases the refractive index n we fortunately obtain
tion p–i–n structure (Fig. 11.88) suffers from enormous an optical waveguide: a central higher-n material em-
carrier leakage and the lack of a medium guiding the bedded in a lower-index material (Fig. 11.89c). Thus,
generated light. To enable operation at room temperature the laser-active layer is the core layer of the waveguide
and considerably reduce the threshold currents at least at the same time. By a proper design, essentially of
a double heterostructure (heterojunction p–i–n structure) the refractive index differences and dimensions, we can
is required (Fig. 11.89). This Nobel-prize-winning idea efficiently guide the generated light in a fundamental
by Koemer and Alferov [11.1257, 1258] enables carrier mode (see the profile in Fig. 11.89c) similar to a single-
confinement and optical confinement by a single impor- mode optical fibre. Considering an edge-emitting laser,
tant modification: using higher-bandgap E g materials the structure is now p–i–n doped and forward-biased
for the p and n regions compared to the central intrin- (Fig. 11.89d), enabling the carrier transport described
sic active layer. Thus, for semiconductor lasers at least above: hole injection from the left and electron injec-
two different materials are required, as shown in space tion from right. The band structure (Fig. 11.89e) of the
z(x, y) (Fig. 11.89a) and in the band structure E(y, z) in doped and biased laser structure visualizes the operation
space (Fig. 11.89b) for an undoped and unbiased struc- of the p–i heterointerface acting as a border (electrical
ture. The central layer (material 1) has a lower E g than confinement) for the electrons. The small potential bar-
the embedding bulk layers (materials 2) and therefore rier at the i–n heterointerface is no real obstacle. The
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 697

electrons can tunnel through or thermally jump across. semiconductor lasers, however, include quantum wells
In analogy, the p–i heterointerface is no real obstacle (QWs, a 2-D carrier system) [11.1259] or quantum dots
for the holes, whereas the n–i heterointerface provides (QDs, a 0-D carrier system) [11.1260] as the laser-active
the required border (electrical confinement). Modern medium, instead of a 3-D laser-active region in bulk

a) d)

Part C 11.3
i i i p i n

Material Material Material


2 1 2

y
z

b) Undoped, unbiased e) Doped, biased

EC

EF

EV

Energy E

y
z

c) f)

n
Intensity

y
Guided
light field

Fig. 11.89a–f Undoped and unbiased (a,b) and doped and biased (d,e,f) separate confinement heterostructures, (a,d)
schematic layer structure in space, (b,e,f) the corresponding band structures in space. The laser active layer is either 3-D
(e) or 2-D (f). (c) refractive-index profile and the fundamental guided mode for the cases (a-d)
698 Part C Coherent and Incoherent Light Sources

Fig. 11.90 Schematic of a semiconductor laser with 3-D


laser-active layer and buried waveguide. Insets: refractive
index profiles and mode profiles in the x- and y-directions
intersecting the active layer at A and B, respectively
Cross si
section B lasers (Fig. 11.89e). In Fig. 11.89f two QWs are depicted
p as an example, providing the emission energy as the dif-
Part C 11.3

A si ference between the energetically lowest bound states in


i
y the wells (note that the ordinate indicates the electron
n energy).
x
z Finally, electrical and optical confinement in the y-
direction (Fig. 11.89c) has to be completed by electrical
B
and optical confinement in the x-direction (Fig. 11.90).
Mode profile Note that this figure is rotated by 90◦ with respect to
Refractive Fig. 11.89. In Fig. 11.90 the active material is embed-
index Cross section A
ded in the x-direction by semi-insulating (si) material
to force the current to move mainly in the active layers
(lateral electrical confinement). The si material is cho-
Energy (eV) sen to have a higher bandgap, and thus a lower refractive
0
a) hh1
Well band edge b) 4 nm GaAs/Al0.15Ga0.85As index, than the active material (lateral optical confine-
–0.02 hh1 ment). Also in this case, wave guiding is applied in the x-
Bulk effective
lh1 masses m *hh, m*lh and z-directions. This is shown in the two insets by the
–0.04 lh1 two cross sections A and B, showing the refractive-index
hh2
profiles and light-intensity profiles. Here, waveguiding
–0.06 in fundamental mode is shown for the case of bulk 3-D
hh3
hh2 active layers.
–0.08
lh2 Barrier band edge 4 nm Well band edge
–0.1 hh1 11.3.2 Resonator Types
and Modern Active Layer Materials:
–0.12 lh1 Quantum Effects and Strain
AlGaAs GaAs AlGaAs
–0.14 hh2 Barrier band edge
8 nm GaAs/Al0.15Ga0.85As Modern optoelectronic semiconductor devices are based
on a sequence of materials of different composition. Em-
0
c) 8 nm GaAs/Al0.3Ga0.7As d) Well band edge hh bedding a film of lower E g between a material of larger
–0.02 hh1
E g , we obtain quantization effects if the film thickness
hh1 L y is on the order of the electron wavelength or below
lh1 Well band edge lh
–0.04 (QW) [11.1259]. Using the Schrödinger equation, we
lh1
obtain at least one bound state in the CB and VB poten-
–0.06 tial wells, respectively. The electrons and holes are still
hh2 hh2
fully mobile in the x- and z-directions. This means that
–0.08
hh3 a wavevector k|| parallel to the heterointerfaces exists.
hh3
The motion in the y-direction is considerably restricted
–0.1
and statistically described by quantum mechanics. Fig-
–0.12 lh2
QW compression = 0.36%
ure 11.91 displays the VB structure in k-space [E(k )]
obtained by a theoretical model calculation [11.1261]
–0.14 8 nm In0.05Ga0.95As/Al0.15Ga0.85As
based on the Schrödinger equation for four different
Ga(In)As/(Al)GaAs QWs (k is oriented parallel to the
0 0.02 0.04 0.06 0.08 0.1 0 0.02 0.04 0.06 0.08 0.1
In-plane wave vector K|| (2ð/a0)
heterointerfaces).
In most cases in addition the QWs and the barriers in
Fig. 11.91 Valence-band structure E(k ) of various Ga(In)As/AlGaAs the active layer are additionally strained [11.1262]. Usu-
QWs [11.1261] ally, the wells are compressively strained, which means
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 699

a) D (E) a) Quantum dot

3D WL WL

2 Substrate
(kx2 + ky2 + kz2)

Part C 11.3
E= 500 nm
2m* b)
c)
E
b) D (E)
2D
50 nm

d)
2
E= (kx2 + kz2) + Ey
2m*
E1 E2 Ey 50 nm
c) D (E)
e)

1D

2 10 nm
kx2
E= + Eyz
2m*
Fig. 11.93 (a) From the bottom to the top we see in sequence: the
E11 E12 Eyz three top monolayers of the GaAs substrate, above two compres-
sively strained monolayers InAs (wetting layer, WL), and above the
d) D (E)
main part of the QD. (b) AFM surface profile of InAs QDs (bright
dots). (c,d) TEM micrograph of a double stack of QDs: (c) stack
0D
distance 40 nm with uncorrelated dots and (d) stack distance 20 nm
E = Exyz with vertically aligned dots ((a-d) [11.1261]). (e) TEM micrograph
of a CdSe QD (dark) in a ZnSe matrix (bright) [11.1263]

Strain and quantization effects in the active layers


E111 Exyz of semiconductor lasers are used to improve the device
properties. For the laser it is beneficial to make the effec-
Fig. 11.92a–d Density of states D(E) and corresponding tive masses of electrons and holes as similar as possible,
formula of the band structure in parabolic approximation to increase material gain, to reduce threshold, to tailor
for a (a) semiconductor extending in all three spatial direc- the density of states and to increase differential gain.
tions (3-D), (b) quantum well (QW), (c) quantum wire, and This can be obtained by applying strain and/or quantiza-
(d) quantum dot (QD) tion. In Fig. 11.92, the energy dependence of the density
of states is shown for 3-D material to be root-like, and
that the lattice constant of that layer is compressively to be constant for 2-D material.
reduced in the x- and z-directions to match that of the Figure 11.93 depicts examples of InAs [11.1263]
substrate ao . In many cases, the barriers are in tension, and CdSe [11.1264] QDs. Schematically, Fig. 11.93a
which indicates that the lattice constant of the barriers shows the QD formation in a cross section of the crys-
is increased in the x- and z-directions by tensile strain tal structure. We see the three upper monolayers of the
to be identical to the substrate lattice constant ao . GaAs substrate. During the self-organized QD formation
700 Part C Coherent and Incoherent Light Sources

the intentionally integrated strain (detailed explanation we obtain a 1-D carrier system and, thus, a quantum
below) of the InAs versus GaAs plays an important wire [11.1265] with hyperbolically shaped density of
role. For thermodynamical and elastomechanical rea- states branches. Limitation of carrier movement in all
sons, two monolayers of strained InAs are first formed. three space directions results in quantum dots [11.1260,
Continuing the growth, for total-energy reasons, it is of 1261, 1263–1272], i. e., a zero-dimensional (0-D) car-
considerable advantage for the semiconductor surface to rier system with a δ-like density of states (Fig. 11.92d).
continue by a localized island-like growth. In this case For many physical properties of the semiconductor (e.g.,
Part C 11.3

a possible geometric shape is a pyramid with a base carrier mobilities, carrier capture in quantized states and
plane directly joined to the top of the InAs monolay- spontaneous or stimulated emission of light), the density
ers. Experimentally, this phase can be directly studied of states plays an important role. Using dimensionality
using an atomic force microscope (AFM) [11.1260]. and strain efficiently during the design of lasers en-
Figure 11.93b displays in a top view a typical AFM ables one to enhance desired and suppress undesired
surface profile. In the next process step the QDs are properties. Here, modern epitaxy [e.g., metal organic
overgrown by GaAs and thereby embedded. Experi- chemical vapour deposition (MOCVD) and molecular
mentally the final layer sequence can be studied by beam epitaxy (MBE)] are powerful tools. To date 2-D
transmission electron microscopy (TEM) after cleaving. and 0-D structures have been used successfully for laser
In order to increase the number of QDs in the direc- devices. 1-D structures have not yet had a breakthrough
tion perpendicular to the substrate interface, the whole due to their disadvantageous dynamic properties. QDs
InAs process is repeated as often as desired after a de- are grown today using self-organization in the Stranski–
fined GaAs spacer layer thickness. This provides layered Krastanow growth mode [11.1263,1265,1267,1271]. By
QD arrangements. Figures 11.93c, d show TEM micro- growing a large number of QDs with identical quantized
graphs for two different spacer-layer widths: 40 nm ad energy levels in the laser-active layer, we would bene-
20 nm. We observe a vertical correlation of the dots fit from a strongly reduced temperature sensitivity and
for the smaller separation. At very high magnification a very high differential gain and, thus, extremely high
Fig. 11.93e shows QD formations in the II/VI semicon- bit rates in optical communication. Although many QD
ductor system CdSe/ZnSe; note the different scales in lasers have been implemented, the pyramid-like QDs
the subfigures. This high TEM magnification resolves suffer from strong fluctuations in size and thus in their
the individual crystal layers. The CdSe QD is contrasted energy levels.
dark against the surrounding brighter ZnSe. On the basis of these QDs, however, the aforemen-
However, quantization is not limited to a single di- tioned improvements in device properties have not yet
rection. If we limit the carrier movement in another be demonstrated. On the other hand, the strong fluctua-
direction (e.g., in the z- and y-direction as in Fig. 11.92), tion causes a strongly spectrally broadened gain profile,

Band gap (eV)


6 AlN Direct semiconductor 0.2
Indirect semiconductor

ZnS
0.35
SiC GaN
ZnSe
3 0.4
AlP AlAs CdS ZnTe 0.5
GaP
2 0.6
AlSb CdTe 0.7
GaAs InP 0.8
Si 1
1 InN 1.3
GaSb 1.55
Ge
GaInAsN InSb
2 Wavelength
GaInAsN InAs 5 (µm) Fig. 11.94 Bandgap energy E g (left)
0
0.3 0.32 0.34 0.36 0.54 0.56 0.58 0.6 0.62 0.64 and bandgap wavelength (right) as
Lattice constant a (nm)
a function of the lattice constant a
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 701

which is beneficial for other applications, e.g., short- (E g = 1.43 eV) and Ga0.47 In0.53 As (E g = 0.75 eV) have
pulse generation by mode locking or wide spectral the same lattice constant as InP (E g = 1.34 eV), which
tuning of the laser device. However, we should also is available in wafers today up to a diameter of 150 mm.
remember that 10 years were necessary after implement- QW widths (or QD dimensions), effective masses
ing the first QW lasers to demonstrate that QW lasers [more precisely the E(k) functions], and bandgaps of
were superior to bulk lasers. Similarly, QD lasers will well and barrier materials energetically determine the
require time before their final breakthrough. However, quantized states and, thus, the spectral gain profile of

Part C 11.3
we believe that QW and QD lasers will share the ap- the laser, i. e., the possible range of laser emission. Fig-
plication area in the future, depending on the specific ure 11.94 shows that a very large wavelength range can
requirements. be covered for different applications. Some examples
Figure 11.94 shows the dependence of the bandgap are red and blue lasers which are used for data stor-
on the lattice constant for various III/V and II/VI age in digital versatile and blue-ray discs, respectively.
semiconductors. The brown area corresponds to the qua- Emission at about 850 nm is used for short-range opti-
ternary Alz Ga1−x−z Inx N. The grey area describes the cal fibre communication and CD devices, 980 nm lasers
quaternary Ga1−x Inx As1−y Py . For high laser efficien- for pumping Er-doped fibre amplifiers, while between
cies in interband lasers, active materials with a direct 1.25 and 1.65 µm the lasers are applied in ultrahigh-bit-
bandgap are required, disregarding for the moment some rate long-haul optical fibre communication. Visible and
intraband lasers. Note that simple bulk Si has an indirect infrared wavelengths are very attractive for optical sens-
band structure and does not provide efficient radiative re- ing. The range between 0.8 and 1 µm is used for direct
combination. Modified Si structures have demonstrated laser applications (welding, drilling, cutting and solder-
strong luminescence, LED operation or laser oscillation, ing) since it includes lasers with extremely high output
e.g., from Si/Ge superlattices, QDs in Si and Si- power, highest wall-plug efficiencies and lowest price
based Raman laser structures [11.1273]. All compound per watt of optical power.
semiconductors, located on one of the grey vertical Stimulated emission and optical gain (Fig. 11.95)
lines (Fig. 11.94) that indicate the lattice constant of are essentially determined by the product of the re-
important semiconductor substrate materials, can be duced electronic density of states and the Fermi factor
lattice-matched to the respective substrate. Accord- ( f c − f v ). This Fermi factor originates from f c (1 − f v ) –
ing to Fig. 11.94 the ternary compounds Al0.48 In0.52 As f v (1 − f c ), namely the probability of processes photon-

fc – fv fc – fv Dred, 2D
Dred, 3D

Optical-gain g (E)

Spontaneous
emission

a) Eg ÄEf E b) Eg Eg' ÄEf E


Absorption

c) E d) E

Fig. 11.95a–d Profile of optical material gain, spontaneous emission, Fermi factors and the density of states as a function
of energy for (a) 3-D und (b) 2-D materials. Corresponding net gain profiles in (c) and (d)
702 Part C Coherent and Incoherent Light Sources

generating photons (emission), i. e., the probability that the net gain can support the modes (vertical lines) as indi-
the CB states are occupied by electrons and VB states are cated. In Fig. 11.95 the spontaneous emission is shown
not occupied by electrons f c (1 − f v ) minus the probabil- by the thin broken lines, revealing a different spectral
ity of processes destroying photons (reabsorption), i. e., profile, which is important, e.g., for LEDs.
the probability of VB states occupied by electrons and Figure 11.96 depicts a classification summary of the
CB states not occupied by electrons f v (1 − f c ). The full most important semiconductor laser geometries. Most
lines in Fig. 11.95a, b schematically show the spectral of them will be treated in detail below. Generally, the
Part C 11.3

material gain profile of 3-D and 2-D semiconductors, heterointerfaces are located horizontally. We distinguish
respectively. Gain ranges spectrally from the bandgap between horizontal (left) and vertical (right) resonator
E g to the difference between the two quasi-Fermi lev- structures, which is indicated by the orientation of the
els ∆E F . In reality there are additional effects such as broad brown double arrow. Thus, we have horizontal
Fermi-level filling, profile broadening [11.1261] (bold cavity lasers (in-plane lasers) and vertical cavity (VC)
broken line) or many-body effects. Material gain minus lasers.
loss provides net gain (Fig. 11.95c, d). If these laser-
active materials are placed in a Fabry–Pérot (FP) laser First case: Fabry–Pérot (FP) structures. Here the opti-
cal reflection (feedback) is provided by the borders of
a) Horizontal cavity b) Vertcal cavity (VC)
the resonator (facets). In many cases, the high refractive
index difference between the semiconductor and the air
is already sufficient, providing an optical reflection co-
efficient of about 30%. By additional facet coatings this
coefficient can be tailored continuously between 0% (an-
tireflection) and 100% (perfect reflection). The resonator
modes are given by
FP DFB  
λB
m FP =L. (11.92)
2n eff
Intuitively, the resonator length L has to be a positive
High facet Low facet integer multiple of half of the wavelength of light in
reflectivity reflectivity the medium, where n eff is the effective refractive index
desired desired DBR 2 (eigenvalue of the Helmholtz equation, see below) of the
waveguide. In the second case, in so-called structures
Cavity
with distributed feedback (DFB), the optical reflection
Edge Surface is extended over the whole resonator. A very efficient
emitter DBR 1
emitter feedback occurs at the Bragg wavelength λB , which is
correlated with the DFB grating period Λ via the Bragg
VCSEL condition:

m DFB (λB /n eff ) = 2Λ . (11.93)

m DFB is a positive integer and describes the grating


DBR laser order. An example: for a DFB laser emitting at λB =
(2nd order) 1.55 µm having a first-order grating (m DFB = 1) and an
effective refractive index n eff = 3.27, a grating period of
Λ = 237 nm is required. Intuitively, an integer multiple
of the wavelength in the medium has to correspond,
according to (11.93), to the double grating period. Note
External that the mathematical structure of (11.92) and (11.93) is
resonator
identical. In lasers with a typical length of 200 µm we
obatin for FP laser modes within the gain profile a very
Fig. 11.96 Different geometries of lasers with horizontal (left) and large m FP (on the order of 1000) while for DFB lasers
vertical resonators (right) in most cases m DFB is 1 (for a first-order grating).
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 703

As expected, light is emitted in horizontal directions can be obtained by an injection of electrons and holes
for edge-emitting lasers (Fig. 11.96). Surface emitters via a forward-biased pn junction (see Figs. 11.89, 90).
can be implemented by etching an out-coupling mirror The electrons injected into the n semiconductor as well
inclined at 45◦ or by a second-order DFB grating (note as the holes injected into the p semiconductor diffuse to
the doubled grating period in the figure). In a second- the pn junction and can recombine there radiatively and
order grating the light field is reflected back horizontally generate a photon with energy ω (Fig. 11.88). If the
(180◦ ) and coupled out vertically. If the Bragg con- external voltage is increased and the carrier density ex-

Part C 11.3
dition is exactly fulfilled, the emission occurs exactly ceeds a critical value in the range of 1018 cm−3 , the rate
perpendicular to the surface (90◦ ). However, the larger of photon emission becomes higher than the absorption
the deviation in (11.93) in the (>)-direction or (<)- rate, so that an incident wave can be amplified coher-
direction, the larger or smaller the angle, respectively. If ently due to stimulated emission. The condition for this
the grating is interrupted we have a distributed Bragg re- population inversion is that the separation between the
flector (DBR) structure. Typically, a central grating-free quasi-Fermi levels E f c and E f v , which describe the fill-
section is embedded between two DBR sections. In the ing of the conduction and valence bands, is larger than
DFB and DBR structures the horizontally propagating the bandgap E g (Bernard–Durafourg condition):
light field alternatively passes two virtual quasi-layers of
E fc − E fv ≥ ω ≥ Eg . (11.94)
slightly different refractive index. For DBR resonators
with real layers (see Sect. 11.3.4 or the next section) In this case the semiconductor material is transpar-
these operation principles become more evident. ent for the generated wave with the wavelength defined
by the bandgap. The resulting gain values are very high
Second case: VCSELs. They are also based on DBR (in the range of 103 cm−1 ) due to the high carrier den-
structures, which in contrast to the first case consist of sity. Lasing occurs if the additional losses of the optical
real multiple layers having a very high refractive-index resonator providing the feedback are compensated.
difference. The central cavity has no grating and is em-
bedded between two DBR mirrors, thus also forming an Double-Heterostructure Lasers
FP-like structure. However, feedback is distributed over The active region, where population inversion is
the two DBR structures. In most cases the thickness achieved, is very thin in homojunction lasers and the
of a single period (equivalent to a pair of neighbor- threshold current is very high, since only a small portion
ing layers) is chosen to equal half the wavelength of of the injected carriers is utilized for the lasing pro-
light in the medium for the design wavelength. This cor- cess. Lower threshold currents and continuous operation
responds to a first-order grating according to (11.93). at room temperature can be achieved with double-
Since the resonator is oriented perpendicularly and the heterostructure lasers, where the low-bandgap active
emission occurs perpendicular to the main chip surface layer is sandwiched between n- and p-doped cladding
(oriented parallel to the substrate area), this laser is called layers with a higher bandgap epitaxially grown on a sub-
a vertical-cavity surface-emitting laser (VCSEL). The strate (Fig. 11.89). The technical realization of these
two mirrors must have a very high reflectivity to reach structures is possible if the lattice mismatch between the
the laser threshold, since the laser-active layer is rela- different layers of the material system does not exceed
tively thin and has a weak overlap with the light field in a critical value. Double heterostructures [11.1257] have
the resonator. three main advantages with respect to laser operation:
Edge-emitting lasers as well as VCSELs will be
treated in detail in the following sections. On the ba- • The bandgap difference between the layers is dis-
sis of both cases (A and B), it is possible to implement tributed between the valence and conduction bands
lasers with external resonators, as indicated in the last and creates potential barriers for the injected elec-
row of Fig. 11.96. trons and holes. For an appropriate choice of doping
and applied voltage, a nearly rectangular-shaped
11.3.3 Edge-Emitting Laser Diodes potential well can be achieved (Fig. 11.89), which
with Horizontal Resonators efficiently confines the carriers in the low-bandgap
active layer if the potential difference is higher than
As already mentioned, the population inversion between the thermal activation energy kB T . The width of the
the valence and conduction bands, which is necessary active layer dact is defined by the heterostructure ge-
for the coherent amplification of radiation [11.1274], ometry. The carriers injected via the pn junction are
704 Part C Coherent and Incoherent Light Sources

captured in the potential well and confined to a small


Confinement factor Ã
volume, thus decreasing the injection current, which 1
3.5
is necessary to achieve inversion.
• There is no reabsorption of the radiation emitted 0.8 n = 3.5
d
3.2
from the active layer in the surrounding layers due
to the difference in bandgap energies. 0.6
• In the material systems used for semiconductor
Part C 11.3

lasers, the low-bandgap active layer has a higher 0.4


refractive index than the surrounding cladding lay-
ers. Therefore, the double heterostructure acts as 0.2
a dielectric planar slab waveguide, confining the ë = 1550 nm
generated optical field to the active region due to 0
the refractive-index difference between the layers. 0 200 400 600 800 1000
Thickness d (nm)
The number of modes supported by this optical
waveguide for a given wavelength depends on the Fig. 11.97 Dependence of the optical confinement factor Γ
thicknesses and the refractive indices of the lay- on the thickness d of an InP/InGaAsP/InP layer structure
ers. By a proper choice of the design parameters,
a single transverse (perpendicular to the pn junc- the waveguide, the confinement factor approaches 1 and
tion) mode can be selected, which concentrates the additional modes are supported.
photon density for stimulated emission in the gain An optical mode with an effective refractive index
region. n eff experiences an effective gain geff in a waveguide
with an active layer, which provides the material gain
Thus, a double heterostructure enables the confinement
gact and has a refractive index n act
of carriers and generated photons in the active layer. For
bulk active layers, the de Broglie wavelength of the car- n act
geff = Γact gact . (11.96)
riers is small compared to the thickness of the active n eff
layer, leading to a high degree of carrier confinement.
The correction factor n act /n eff takes into account the
The wavelength of the photons, however, is comparable
waveguiding effect on the modal gain [11.1275].
to the dimension of the structure, so that only a portion of
the optical intensity is confined to the active region. The
Laser Structures
transversal distribution of the light intensity in the dou-
Using modern epitaxial growth methods it is possible
ble heterostructure is given by the solution of the wave
to realize semiconductor multilayer structures very pre-
equation of a planar slab waveguide supporting TE and
cisely so that stable, transverse single-mode operation
TM modes with an effective index n eff as the respective
can be obtained using dielectric waveguiding [11.1276].
eigenvalue. Figure 11.89c shows the optical intensity of
For most applications, however, lateral (parallel to the
the fundamental TE mode in a double heterostructure as
pn junction) patterning of the laser structure is also re-
a function of the transversal coordinate y, revealing the
quired to obtain lateral carrier and photon confinement,
incomplete confinement of the optical field in the active
which is important to obtain stable and efficient laser
region. The fraction of the mode intensity within the ac-
operation with high spectral purity and good coupling
tive layer is called the optical confinement or the filling
efficiency into a fibre. In addition, lateral confinement of
factor Γact , which is an important design parameter for
the injection current is necessary to avoid leakage cur-
a semiconductor laser:
 dact rents bypassing the active region. The confinement of
|E(y)|2 dy photons, carriers and current has been implemented in
Γact =  0+∞ , (11.95) many ways, reflecting the specific purpose of the de-
−∞ |E(y)| dy
2
vice. Semiconductor lasers can be classified according
where E(y) is the electric field. If the light is also con- to the mechanism of lateral waveguiding as gain-guided
fined in the lateral direction of the laser, the definition or index-guided, depending on whether it is the lateral
has to be modified accordingly. variation of the optical gain or the refractive index that
The dependence of the optical confinement factor of confines the mode. Index-guided lasers can further be
the guided modes on the thickness d for a layer struc- subclassified as weakly or strongly index-guided, de-
ture is shown in Fig. 11.97. For increasing thickness of pending on the magnitude of the lateral refractive-index
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 705

Gainguiding Indexguiding
Laserstructure Oxide stripe laser Buried active layer
w w

p-contact Isolator p-contact Isolator

p d p

Part C 11.3
Active layer n < nact
y n n

n-contact n-contact
x

P– I curve
P (mW) P (mW)

– “Kinks” due to unstable


10 lateral waveguiding 10
Stable, lateral monomode
– Threshold high and not operation with low threshold
5 clearly defined due to strong 5
spontaneous emission
0 0
0 50 100 150 0 50 100 150
I (mA) I (mA)

Spectrum
Intensity (arb, units)) Intensity (arb, units))
1 1
0.8 0.8
0.6 Multimode due to 0.6 Few modes due to
strong spontaneous weak spontaneous
0.4 emission 0.4 emission
0.2 0.2
0 0
1.52 1.525 1.53 1.535 1.54 1.52 1.525 1.53 1.535 1.54
Wavelength (µm) Wavelength (µm)

Farfield
Intensity (arb, units)) Intensity (arb, units))
1 1
0.8 0.8
0.6 0.6
0.4 0.4
0.2 0.2
0 0
–40 –20 0 20 40 –40 –20 0 20 40
Angle è|| (deg) Angle è|| (deg)

Phase fronts
Curved Planar

w w

x x

z z

Fig. 11.98 Comparison of gain-guided and index-guided laser structures


706 Part C Coherent and Incoherent Light Sources

step. In a gain-guided laser structure (oxide stripe laser, two categories: ridge waveguide lasers and channeled
Fig. 11.98, left) the current is injected via a stripe con- substrate lasers.
tact (width w ≈ 5 µm) in a laterally unpatterned active In ridge-waveguide lasers, a rib waveguide is de-
layer. The optical field is mainly guided by the result- fined by etching a narrow stripe (≈ 3–5 µm) down near
ing variation of the gain. The lateral waveguiding is to the active layer (at a typical distance of 200 nm). In the
weak, so that even small variations of the refractive case of a metal-clad-ridge waveguide (MCRW) laser in
index, e.g., due to temperature changes or carrier in-
Part C 11.3

jection lead to unstable operation. In an index-guided


laser structure (buried laser structure, Fig. 11.98, right) a) Metal-clad-ridge waveguide (MCRW) laser
4 µm
the active layer (w ≈ 2 µm) is laterally embedded into
a material with a lower refractive index (n < n act ), higher Cr-Au electrode
bandgap and higher electrical resistivity to facilitate sta-
p+- GaAs
ble lateral waveguiding, carrier confinement and current
confinement. The typical features of index- and gain-
guided laser structures are summarized in Fig. 11.98. p-AlGaAs
GaAs (active)
The power–current characteristic (P–I curve) of gain-
guided lasers is characterized by a high threshold current n-AlGaAs
(typical 50–100 mA) and kinks originating from the
unstable lateral waveguiding. The optical spectrum is
multimodal due to the enhanced spontaneous emission. n-GaAs substrate
The phase-fronts are curved in the resonator and the far
field shows the characteristic twin lobes caused by the AuGeNi elektrode
laterally inhomogeneous gain distribution. The main ad-
vantage of gain-guided lasers is the simplicity of their b) Ridge waveguide laser
4 µm
fabrication. For very large stripe widths (50–100 µm)
a so-called broad-area laser results, in which the cur- p contact
rent is injected laterally and homogeneously via a large
p-InGaAsP
contact. Since there is no lateral waveguiding in broad-
SiO2
area lasers, the threshold current is very high (typical
a few A) and the multimode emission cannot be coupled p-InP
InGaAsP (active)
efficiently into a fibre. Due to the high output power,
broad-area lasers are used, e.g., for optical pumping of n-InP
solid-state lasers.
Index-guided lasers show stable, lateral single-mode
emission with a low threshold current (typical 10 mA) n-InP substrate
and a P–I curve without kinks. The spontaneous emis-
sion in each mode is significantly smaller, resulting in n contact
a spectrum with a few dominating modes. The phase-
c) Channeled-substrate planar (CSP) laser
fronts are planar and the far field has a smooth shape,
2 µm
enabling a high coupling efficiency into a single-mode
AuZn electrode p+-Zn diffusion
fibre.
nGaAs
p-Al0.6Ga0.4As 0.05 µm
Weakly index-guided laser structures. In weakly
p-Al0.15Ga0.85As (aktiv)
index-guided lasers the thickness of the waveguiding n-Al0.6Ga0.4As
layer is varied, thus resulting in a lateral waveguiding 1.5 µm
0.3 µm
structure. Lateral single-mode emission can be ob-
tained by a proper choice of the thickness and width
of this variation. The lateral index step has to exceed n-GaAs substrate
the carrier-induced reduction of the refractive index
AuGe electrode
(∆n ≈ 5 × 10−3 ) so that index-guiding is dominating.
Weakly index-guided laser structures can be divided into Fig. 11.99 Weakly index-guided laser structures
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 707

the material system GaAlAs (Fig. 11.99a) a CrAu elec- nearly planarized, thus generating a lateral waveguiding
trode is deposited, which gives an electrically conductive structure, since the active layer has a higher refractive
contact on the p+ top layer of the rib and an insulat- index. Current bypass can be reduced by guiding the
ing contact on the p-GaAlAs layer with lower doping injection current using, e.g., localized Zn diffusion.
along the rib. Thus, the current injection is focused in Weakly index-guided lasers are suitable to obtain
the region of the active layer below the rib. This current low threshold currents of typically 20–40 mA and high
confinement can also be realized by additional isolating output powers with lateral single-mode emission. The

Part C 11.3
layers, e.g., SiO2 (Fig. 11.99b). The lateral waveguid- weak waveguiding allows for broader active layers com-
ing is accomplished by the higher refractive index of pared to buried laser structures, which has a positive
the semiconductor material compared to the surround- effect, e.g., on the series resistance. The low current
ing SiO2 and air. The etch depth has to be carefully leakage in ridge waveguide lasers usually results in good
controlled (e.g., by using etch-stop layers) in order to linearity of the P–I curve. The emission is more com-
select one lateral mode and minimize current bypass. plex than in buried lasers, since index- and gain-guiding
The first step in the processing of channeled sub- are important and even small changes of the refractive in-
strate lasers is the etch of a 2–3 µm-wide and 1 µm-deep dex by temperature or current injection can influence the
channel into the substrate (Fig. 11.99c). In the subse- performance. The active layer in weakly index-guided
quent epitaxy (e.g., liquid-phase epitaxy) this channel is lasers is not affected during processing, so that lateral

a) Buried heterostructure (BH) laser b) Etched-mesa buried heterostructure (EMBH)


4 µm 2 µm

AuZn SiO2 p contact

+ p-InGaAsP
p - GaAs
n-AlGaAs
p-AlGaAs
n-InP p-InP
p-AlGaAs GaAs (active)

n-AlGaAs
p-InP
InGaAsP (active)
n-InP

n-GaAs-substrate n-InP substrate

AuGe n contact

c) Double-channel planar buried heterostructure d) Mushroom laser


(DCPBH) laser
3 µm 6 µm

AuZn SiO2 SiO2 AuGe/Au

p+-InGaAsP n-InP
s.i.-InP 3µm
p-InP n-InP
p-InP
p-InP
p-InP
p-InP p-InP
p-InP InGaAsP (active) InGaAsP (active)

n-InP substrate
p-InP substrate

AuGe AuZn contact

Fig. 11.100 Buried heterostructure lasers


708 Part C Coherent and Incoherent Light Sources

carrier diffusion in the active layer cannot be avoided, but ical etching process the width of the active region is
on the other hand, the unpatterned active layer is advan- reduced up to 1–2 µm to obtain lateral single-mode op-
tageous for the reliability of the device. Since only one eration. The resulting undercut area is epitaxially refilled
epitaxial growth step is needed, the fabrication of these afterwards, e.g., using vapor phase epitaxy (VPE) with
lasers is significantly easier than buried semiconductor semi-insulating InP [11.1279].
lasers. In addition to this strongly index-guided laser struc-
tures with a planar active layer, which are useful for
Part C 11.3

Strongly index-guided laser structures. Strong index- integration with a DFB grating, there also exist buried
guiding can be accomplished by buried laser structures, laser structures utilizing nonplanar active layers based
where a small stripe of the active layer material with on the regrowth of, e.g., V-grooves or mesas.
a high refractive index is embedded into semiconductor Using strongly index-guided structures, a very sta-
material with lower refractive index and larger bandgap. ble and lateral single-mode laser operation with very low
For this purpose, the active layer has to be patterned threshold currents (< 10 mA) and excellent high-speed
and epitaxially regrown afterwards. Lateral single-mode characteristics can be obtained, since stable optical
operation is possible, if the resulting stripe width of the waveguiding, carrier confinement and current confine-
active layer does not exceed a critical value defined by ment are combined. The fabrication of these devices,
the cut-off for the higher lateral modes [11.1277]. however, is complicated due to the additional epitaxy
Figure 11.100 shows some examples for strongly step.
index-guided laser structures. In the case of a buried-
heterostructure (BH) laser structure in the material Edge-emitting Fabry–Pérot laser diodes
system GaAs/GaAlAs (Fig. 11.100a) the GaAs active In Fabry–Pérot (FP) lasers, the cleaved facets of the
layer is surrounded by AlGaAs, which has a larger semiconductor crystal form the optical resonator, which
bandgap and a lower refractive index. The active layer enables laser operation by providing the optical feedback
is grown in the first epitaxial step and structured into of the stimulated amplified radiation. This resonator se-
1–2 µm-wide stripes. Using liquid-phase epitaxy (LPE), lects the photons generated by stimulated emission with
which planarizes the structure, the regions alongside respect to direction and wavelength. The light wave trav-
the stripe are refilled with alternating n- and p-doped eling perpendicularly to the facets is amplified if the
AlGaAs layers. This reverse-biased diode structure pre- wavelength matches a longitudinal mode of the res-
vents the current from bypassing the active region. In onator [(11.92), Figs. 11.90, 95, 96, 103a]. The lasing
a similar way, a BH structure can be realized in the process starts if the gain experienced during one round-
long-wavelength material system InGaAsP/InP (Etched- trip in the cavity equals the losses caused by absorption,
mesa buried heterostructure laser, Fig. 11.100b). The scattering and the light output through the facets.
reduction of leakage current using alternating n- and
p-doped layers, however, leads to a significant increase Lasing condition. The length L of the resonator is
of the parasitic electrical capacity of the laser, which typically a few hundred micrometers. The intensity re-
degrades the high-frequency response of the device. Al- flection and transmission coefficients of the end facets
ternatively, electrically isolating regions for the current can be estimated using the Fresnel equations, neglect-
confinement can be fabricated using semi-insulating ma- ing the transversal and lateral structure of the waveguide
terial (e.g., Fe-doped InP) or by proton implantation. In with the air (n = 1) assumed to be outside the cavity:
Double-channel substrate planar buried heterostructure
(n eff − 1)2 4n eff
(DCPBH) lasers (Fig. 11.100c) the first epitaxial growth R= , T= , (11.97)
step produces the active InGaAsP-layer and a p-InP cap (n eff + 1)2 (n eff + 1)2
layer on the n-InP substrate. Then, a double-stripe struc- where n eff is the effective refractive index of the wave-
ture embedding the active region is created by etching. guide mode considered.
In the subsequent LPE step the generated channels are In this one-dimensional model plane waves with
refilled with p-InP/n-InP and the epitaxial growth of the electric field amplitude E(z) travel in the longitudi-
laser structure is finished up to the InGaAsP top layer. nal direction (z) of the FP resonator, experiencing the
The processing of the mushroom laser (Fig. 11.100d) modal intensity gain g due to stimulated emission. The
begins with the etching of 6 µm-wide mesa in the layer threshold for laser operation is defined by a round-trip
structure, which cuts through the active layer grown in condition requiring that in a stationary state the optical
the first epitaxy [11.1278]. Using a selective wet chem- wave remains unchanged after one complete round-trip
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 709

P, N
I (y)
P
n2 n1 Ë w

dact Ãact

Nthr N

Part C 11.3
y
z
Stimulated 0 L
Fig. 11.102 Scheme of a DFB laser structure with an integrated rect-
angular Bragg grating (duty cycle w/Λ) including the corresponding
Spontaneous transversal intensity distribution I (x)
Ithr I
separation ∆ν of adjacent modes is influenced by the dis-
Fig. 11.101 Dependence of the output power (P) and carrier persion of the waveguide, which is taken into account
density (N) on the injected current by the group refractive index n g
c
in the cavity. This round-trip condition gives the mirror ∆ν = (11.100)
losses of the FP resonator 2Ln g

1 with
g = αm = ln(R1 R2 ) , (11.98)
2L dn eff
n g = n eff + ν . (11.101)
where R1 and R2 denote the intensity reflection coeffi- dν
cients of the end facets. Since the net gain g in the cavity For a typical FP laser diode the group index
is composed of the material gain of the semiconductor of n g ≈ 3.5–5 is higher than the effective index
geff and the waveguide losses αs , the lasing condition n eff ≈ 3–3.5. The separation of the equidistant mode
can be written as frequencies is about 150 GHz for a 300 µm-long cavity,
n act which is small compared to the width of the gain curve of
gthr = Γact gact (Nthr ) = αs + αm (11.99)
n eff
if the contribution of spontaneous emission is neglected a)
FP
and Nthr denotes the carrier density at threshold. The 2
Eel
optical losses of the waveguide are caused by optical y
scattering from imperfections in the bulk media or at
z z
interfaces and free-carrier absorption in the active and
cladding layers. b) DFB
The longitudinal distribution of the photon density
s(z) in the active FP resonator is given by the sum of the Stop band
forward and backward traveling photon densities, which
grow exponentially due to the gain g. For a symmetric c) DFB
resonator (R = R1 = R2 ) the total photon density s(z) is
given by a cosh function (Fig. 11.103a) with a minimum Stop band
in the middle of the resonator. For a laser diode with
as-cleaved facets (R = 0.28), the intensity distribution d) VCSEL
is relatively flat, whereas for antireflection-coated facets log intensity
a strongly inhomogeneous photon distribution results.
The round-trip condition also gives the optical fre-
ë
quencies of the longitudinal modes of the FP resonator
according to νq = qc/(2Ln eff ), where q = 1, 2, 3 · · · Fig. 11.103 Schematic structural cross sections (left) and the corre-
and c denotes the vacuum speed of light. The frequency sponding emission spectra (right) for various diode lasers
710 Part C Coherent and Incoherent Light Sources

the semiconductor (≈ 5 THz). Thus, longitudinal multi- number S = sV/Γact via


mode operation can be expected above threshold for an 
FP laser diode. E(t) = S(t) exp[iΦ(t)] , (11.106)
For many applications the degree of single-mode Rsp is the time-averaged rate of spontaneous emission
emission is important; it can be quantified by the side- into the lasing mode; Fs (t), FN (t) and FΦ (t) represent
mode suppression ratio (SMSR): Langevin noise sources taking into account the statistic
nature of the spontaneous emission and the shot-noise
Part C 11.3

SMSR = 10 log10 (P1 /P2 ) , (11.102) character of the carrier recombination and generation.
The Langevin forces leading to fluctuations of carrier
where P1 and P2 ≤ P1 denote the output power of the
density and photon density are correlated and have zero
two strongest modes in the optical spectrum. Typical
mean [11.1280].
FP laser diodes achieve a maximum SMSR of approxi-
The longitudinal excess factor K z accounts for the
mately 20 dB.
enhancement of the spontaneous-emission noise due to
the axial dependence of the complex electric field E(z, t)
Rate equations. The fundamental static and dynamic L
properties of semiconductor laser diodes can be mod- | 0 |E(z, t)|2 dz|2
eled using a set of rate equations [11.1280] describing K z (t) =  L . (11.107)
| 0 E 2 (z, t) dz|2
the interaction of electron–hole pairs and photons in
the active layer. We consider a strongly index-guiding In the case of a transversely single-mode index-guided
double heterostructure supporting a single optical mode FP laser the factor K z is given by [11.1281]
traveling as a plane wave axially in the cavity. The  √ √ √ 2
( R1 + R2 )(1 − R1 R2 )
current I is assumed to be uniformly injected into the K zFP = √ .
active layer with volume V and recombines there, com- R1 R2 ln(1/R1 R2 )
pletely neglecting leakage currents. The carrier density (11.108)
within the active layer is treated as homogeneous in the The first rate equation (11.103) can be formally
transversal and lateral direction, since the correspond- derived from the quantum-mechanical density-matrix
ing inhomogeneities of photon density are small and the formalism. It can be interpreted as a balance of carri-
resulting gradients in carrier density are smoothed out ers that are injected as a current I and contribute to
by diffusion. In FP lasers with a sufficiently high mirror stimulated emission or are lost for the lasing process via
reflectivity, the axial variations of the photon density s the different recombination processes. The second and
and the carrier density N can be neglected and the rate third equations (11.104, 105) can be derived from the
equations can be written as: Maxwell equations with the rotating-wave and slowly
dN I N varying amplitude approximations.
= − − BN 2 − CN 3 For semiconductor lasers with a bulk active layer, the
dt eV τnr
dependence of the gain on the carrier density gact (N) can
n act FN (t)
− vg gact (N, s)s + , (11.103) be approximated as linear [11.1282]
n eff V
 dg
ds n act gact (N) = (N − Ntr ) , (11.109)
=vg Γact gact (N, s) − gthr s dN
dt n
 eff  where dg/ dN is the differential gain and Ntr is the
Γact Rsp + Fs (t)
+ , (11.104) transparency carrier density. In quantum well structures
V (Figs. 11.91, 92) this dependence is usually described by
dΦ 1 n act a logarithmic function [11.1283, 1284]
= αH vg Γact gact (N, s) + FΦ (t) , (11.105)
dt 2 n eff
dg N
gact (N) = N ln for gact ≥ 0 . (11.110)
where vg = c/n g is the group velocity of the waveguide, dN Ntr
e the electron charge, gact is the material gain of the The influence of the photon density on the gain is taken
active layer, Γact is the optical confinement factor of into account by introducing a nonlinear gain coefficient
the active layer and 1/τnr , B and C are the parameters ε according to:
describing nonradiative, bimolecular and Auger recom-
bination, respectively. Φ is the phase of the complex gact (N)
gact (N, s) = . (11.111)
electric field E, which is connected with the photon 1 + εs
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 711

This nonlinear gain compression is caused by spectral small and (11.103) gives a linear increase of the car-
hole burning and carrier heating, which is significant rier density according to N ∝ I/eV . Above threshold
if the time constant of stimulated emission becomes the gain is approximately clamped at g(Nthr ) = gthr and
comparable to the intraband relaxation time. the corresponding threshold current, which is defined
in the limiting case of vanishing spontaneous emission
Refractive index change. In semiconductors the real (Rsp = 0), becomes
part of the refractive index depends on the carrier density  
Nthr

Part C 11.3
because of various physical mechanisms. With increas- Ithr = eV + BNthr
2
+ CNthr
3
. (11.115)
ing injection the band-to-band absorption is reduced due τnr
to band-filling effects. In addition, the absorption in- Using (11.103) the photon number above thresh-
creases due to the reduction of the bandgap (bandgap old can then be written as S = (I − Ithr )/evg gthr . Since
renormalization resulting from many-body effects) and the carrier density is clamped at threshold, all injected
absorption also increases due to the increasing absorp- carriers in excess of the threshold current contribute
tion of free carriers. The resulting total change of the real to stimulated emission and the number of photons in-
part of the refractive index, which is related to the gain creases proportionally to (I − Ithr ). The total output
spectrum via the Kramers–Kronig relation, depends on power P = vg ωαm S emitted from both facets becomes
the wavelength relative to the gain maximum. In the case
ω αm
of 1.5 µm InGaAsP the refractive index decreases with P= ηi (I − Ithr ) , (11.116)
injection. The dependence of the refractive index on the e gthr
carrier density is theoretically described by the effective where we assume that only a fraction ηi of the ex-
line width enhancement or Henry factor α ternal drive current reaches the active region and the
∂n eff remaining fraction (1 − ηi ) is lost via leakage cur-
α= , (11.112) rent or nonradiative recombination. Thus, the P–I
∂γeff
curve of a semiconductor laser diode is a straight line
where the complex effective refractive index is defined (Fig. 11.101) above threshold with a slope defined by
by n eff − iγeff . The change of the effective index with the external quantum efficiency ηext :
carrier density can be written as
dP e αm
n act n act αλ ∂gact (N) ηext = = ηi , (11.117)
δn eff ∼
= Γact δn act = −Γact δN . dI ω gthr
n eff n eff 4π ∂N
(11.113)
which can be interpreted as the ratio of the number
of emitted photons to the number of injected elec-
The line width enhancement factor is important for trons per time. The sharpness of the transition from
the treatment of line width and frequency chirp un- the spontaneous emission below threshold to the stimu-
der modulation [11.1281]. Typically it ranges from 3 lated emission above threshold depends on the amount
to 5, decreasing from the long-wavelength to the short- of spontaneous emission into the lasing mode. Leak-
wavelength side of the gain curve [11.1282]. age currents, thermal effects and spectral hole-burning
neglected so far lead to bending of the P–I curve.
Steady-state characteristics. The single-mode rate
equations can be used to analyze the steady-state behav- Characteristic temperature. The threshold current of
ior of a semiconductor laser. Setting the time derivative a semiconductor laser depends on the temperature T ,
to zero in (11.104), we obtain an implicit expression for which can be described phenomenologically by
the photon number S in the case of continuous-wave
T
(CW) operation: Ithr (T ) = I0 exp , (11.118)
T0
Rsp
S= . (11.114) where T0 is the characteristic temperature, which typi-
vg [gthr − Γact gact (N, s)]
cally ranges between 40 K and 90 K for semiconductor
The number of photons increases as the gain value lasers emitting around 1550 nm.
asymptotically approaches the losses gthr. The small gain
difference is compensated by spontaneous emission, Single-Mode Laser Structures
which provides the noise input amplified by stimu- Transmitters used, e.g., in optical-fibre communication
lated emission. Below threshold the photon density is systems should emit light predominantly in a single
712 Part C Coherent and Incoherent Light Sources

longitudinal mode since the presence of side modes lim- Bragg grating. The method most frequently used to
its the transmission capacity due to pulse broadening achieve single-mode emission is to incorporate a Bragg
caused by the chromatic dispersion of the fibre. Semi- grating, which creates a periodic variation of the
conductor lasers with an FP resonator usually exhibit complex refractive index and distributes the feedback
multimode operation since the gain spectrum is wider throughout the cavity. Dynamic single-mode operation
than the longitudinal mode spacing and the broadening is achieved if the threshold gain for the oscillating
of the gain profile, which due to spectral hole burning is mode is significantly smaller than the threshold gain
Part C 11.3

not perfectly homogeneous, offers several modes with for the other modes. Devices employing Bragg grat-
sufficient gain to oscillate. The techniques to achieve ings can be classified roughly into three categories:
reliable longitudinal mode control even under high- distributed Bragg reflector (DBR), distributed feedback
bit-rate modulation can be categorized into two main (DFB) (Figs. 11.96, 102, 103, section on Fabry–Pérot
groups: structures in Sect. 11.3.2, and Sect. 11.3.6) and gain-
coupled (GC) lasers.
Short lasers. The discrimination against side modes in In DBR lasers the Bragg grating is etched into pas-
FP resonators can be enhanced by reducing the cavity sive regions near the cavity ends. The index grating (the
length L. If the mode spacing ∆ν ∝ L −1 becomes com- variation of the real part of the refractive index) acts as
parable to the width of the gain curve, only one mode an effective mirror with wavelength-dependent reflec-
will oscillate near the gain peak. To obtain stable single- tivity and surrounds the central part of the cavity which
mode operation, however, the lasers must be extremely is active and remains uncorrugated. The longitudinal
short. This requires a very good reflectivity of the end mode with a wavelength located near the reflectivity
facets to overcome the high mirror losses αm ∝ L −1 , maximum of the grating is selected. Since a DBR laser
leading to high threshold current densities. The prob- is formed by replacing the mirrors by passive gratings,
lems of fabricating very short semiconductor devices the properties can be described by an effective mirror
can be solved using a vertical-cavity surface-emitting model. The transition between the active section and
laser (VCSEL) structure (Fig. 11.96). the passive gratings usually complicates the technolog-
ical realization of in-plane DBR lasers. An important
Frequency-selective feedback. The second method advantage of DBR lasers is that the wavelength can be
to obtain single-mode operation is to incorporate changed if the grating regions are equipped with sep-
a frequency-selective element in the resonator struc- arate electrodes that can tune the Bragg frequency via
ture. This can be realized by using coupled cavities, the carrier-induced refractive index change. Thus, DBR
an external grating or a Bragg grating: gratings are often used in tunable lasers.
In DFB lasers the index grating covers the entire
Coupled cavities. If one or more additional mirrors are resonator length. At the wavelength corresponding to
introduced in the FP resonator, the boundary conditions the corrugation period of the grating, the forward- and
added due to the reflections at each interface severely backward-traveling waves created by the Bragg scat-
limit the number of longitudinal modes. To achieve tering are confined in the central part of the cavity so
single-mode operation, however, it is often necessary to that the mirror losses become a function of the wave-
tune the resonator by changing the drive current or the length. The longitudinal mode with the lowest mirror
temperature. Usually the single-mode regime is small so losses corresponding to the most effective concentration
that such structures can only be modulated over a limited of photons in the resonator is selected.
current range without mode jumps. In addition, the re- In gain-coupled devices a periodic variation of gain
producible fabrication of nearly identical devices turns or loss is used to favor a longitudinal mode of the
out to be difficult since the spectral properties strongly FP resonator. In the ideal case, there is no Bragg
depend on the exact lengths of the sections. scattering at the gain grating, and the longitudinal
photon distribution as well as the mirror losses are un-
External grating. Frequency selection can also be real- changed compared to the FP cavity. The overlap with
ized by an external grating outside the resonator. The the loss or gain grating, however, varies between the
mechanical stability of such lasers, however, is a crit- different longitudinal modes of the FP resonator. The
ical point since the grating is not integrated on the mode experiencing the largest overlap with the gain
wafer. Consequently, lasers with external gratings are grating (or minimum overlap with a loss grating) is
expensive devices (Fig. 11.110a). selected.
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 713

DFB lasers. The spectral properties of DFB losses. In addition, the coupling coefficient of second-
lasers [11.1285] are essentially determined by the inte- order gratings depends more sensitively on the exact
grated Bragg grating. The waveguding in such periodic shape of the grating so that it becomes more difficult to
structures can be analyzed by the coupled mode the- control. That is why first-order gratings predominate al-
ory [11.1286], which yields approximate analytical though the corrugation periods are smaller (Λ ∼= 240 nm
solutions describing the light propagation in waveguides for λ = 1.55 µm). Due to the scattering perpendicular
with a periodic variation of the complex refractive index to the optical axis (Fig. 11.96), second-order gratings

Part C 11.3
by counter-propagating modes exchanging energy by can be utilized for the vertical emission of light from
scattering. The strength of the interaction and the amount edge-emitting laser diodes [11.1287, 1288].
of feedback in the grating structure are determined by
the complex coupling coefficient Basic properties of index-coupled DFB lasers. The
spectrum of an index-coupled DFB laser mainly con-
κ = π∆n/λ0 + i∆g/4 , (11.119)
sists of two degenerate lasing modes at the edges of
which is proportional to the variation of the refractive the stop-band (Fig. 11.103b). This mode degeneracy in
index step ∆n, the gain variation ∆g and the number of index-coupled DFB laser structures is usually removed
corrugations per length in the grating. The Bragg wave- by incorporating a λ/4 phase shift in the grating. This
length λB is given by the effective index, the corrugation can technologically be implemented by inserting an ad-
period Λ and the order m DFB of the grating according to ditional section of length λ0 /(4n eff ) = Λ/2 in the middle
(11.93). For an axially homogeneous first-order grating of the grating. The introduction of the λ/4 phase shift
(m DFB = 1) with length L and a perfect antireflection selects the Bragg mode in the middle of the stop-band,
coating on the facets (R1 = R2 = 0) the theory reveals revealing the lowest mirror losses so that single-mode
the following solutions operation with an SMSR of > 40 dB can be obtained
(Fig. 11.103c).
• In the case of pure index coupling (∆n eff =
The axial distribution of the light intensity in the cav-
0, ∆g = 0) the transmission spectrum turns out
ity is connected to the mirror losses αm via the round-trip
to be symmetric with respect to the Bragg wave-
condition. Thus, a decrease of the mirror losses for the
length λB = 2n eff Λ where oscillation is forbidden.
longitudinal modes in a DFB grating is equivalent to in-
For a small coupling coefficient, the mode spacing
creasing longitudinal optical confinement, which means
approximately takes the value of an FP resonator
that the photons are concentrated inside the cavity and
∆λ = λ2 /2n eff L but, in contrast to an FP cavity, the
only a small fraction of the light intensity leaves the res-
threshold gain of the modes is wavelength dependent
onator through the end facets. The typical longitudinal
and increases with growing distance from the Bragg
photon distribution for a DFB laser with and without
wavelength. A strong coupling produces a trans-
a λ/4 phase shift is shown in Fig. 11.103, revealing the
mission stop-band with width ∆λ ∼ = κλ2B /(πn eff )
pronounced maximum in the middle of the resonator
centered at the Bragg wavelength, in which trans-
even for moderate coupling coefficients. This strong in-
mission is strongly damped. The two modes with
homogeneity of the photon density distribution in DFB
the lowest threshold gain g ∼ = 2π 2 /(κ 2 L 3 ) are lo-
lasers leads to an inhomogeneous carrier density dis-
cated at the edges of the stop-band symmetrical to
tribution above threshold due to the recombination by
the Bragg wavelength.
stimulated emission. With increasing injection the car-
• In the case of pure gain coupling (∆g = 0, ∆n eff =
rier density is depleted in places with a high photon
0) the mode degeneracy is removed, which means
density. This phenomenon is called longitudinal spatial
that the mode with the lowest threshold gain os-
hole burning (LSHB) and has several important conse-
cillates at the Bragg wavelength symmetrically
quences for the static and dynamic behavior of DFB
surrounded by the other modes with higher threshold
lasers above threshold. First, the mode discrimination is
gain values. The mode spacing is ∆λ = λ2 /2n eff L
influenced since a variation of the carrier density distri-
and no stop-band occurs since there is no backscat-
bution changes the round-trip gain of the various modes
tering at index steps in the grating. The mode
having different photon density distributions. Thus, the
selection is due to the different overlap of the stand-
side-mode suppression can degrade with increasing out-
ing waves in the FP resonator with the gain grating.
put power due to LSHB. Second, the mode wavelengths
In second-order gratings (m DFB = 2) additional scatter- change, even above threshold, since the inhomogeneity
ing occurs in the transversal direction, leading to higher of the carrier density caused by LSHB leads to an inho-
714 Part C Coherent and Incoherent Light Sources

mogeneous axial distribution of the effective refractive compensated for if the injected current density is
index. This effect is utilized in several types of tunable higher in the central section near the peak of the
DFB lasers. photon density, thus reducing the gain of the side-
Various DFB lasers with a more complex grating modes suffering from the lower current in the outer
structure have been developed in order to obtain a high section [11.1295].
yield of single-mode devices and a flat axial photon
The phase relation between the grating and the end
distribution with reduced LSHB. Some examples are:
facets is difficult to control during the cleaving pro-
Part C 11.3

cess of DFB lasers, since the corrugation period for


• 2 × λ/8 phase shifts. The distance between the phase
a first-order grating (λ = 1.55 µm) is typically 240 nm.
shifts, however, must be optimized to achieve a high
Experimental and theoretical investigations show that
yield [11.1289].
all static and dynamic optical properties of as-cleaved
• Corrugation pitch modulation (CPM). The DFB
DFB lasers are strongly influenced by this phase rela-
grating is divided into three sections. The cor-
tion between the grating and facet. The mirror losses
rugation period in the central section is slightly
of the various longitudinal modes, the mode discrimi-
higher than in the outer sections so that the phase
nation, the intensity distribution, the optical spectra and
shift is quasi-continuously distributed along the cav-
the dynamic and noise characteristics vary considerably
ity [11.1290].
as a function of the end facet phases [11.1296]. Since
• Axial variation of duty cycle by using, e.g., a holo-
these end facet phases are distributed randomly after the
graphic double-exposure technique [11.1291].
cleaving process, the yield of good DFB devices is lim-
• Axial variation of coupling coefficient by vari-
ited. The problem of the uncertain end facet phases can
ation of the etch depth [11.1292] or sampled
be reduced by appropriate antireflection coatings.
gratings [11.1293].
• Bent waveguides superimposed on homogeneous
Gain-coupled lasers. In gain-coupled laser structures,
grating fields can be used to obtain quasi-
a longitudinal mode of the FP resonator is selected by
continuously and arbitrarily chirped gratings with
implementing an axial gain or loss grating. In contrast
high spatial resolution [11.1294].
to index-coupled DFB lasers, there is almost no reflec-
• Axially inhomogeneous injection using a three-
tion of the light wave in a gain grating. Therefore, the
electrode structure. Spatial hole burning can be
longitudinal intensity distribution and the spectral posi-
tions of the various modes are equal to those of an FP
a) Grating layer: Eg > Eg, act
resonator. The mode selection is caused by the different
Än ¹ 0 Ë overlap of the longitudinal modes with the gain grating.
The mode, whose longitudinal field distribution exhibits
the largest overlap with the gain grating or the smallest
overlap with the loss grating, is selected.
dact Gain coupling can be realized in different ways:
Active layer: Eg, act • The grating structure can be etched directly into the
b) Ë active layer and regrown afterwards with a semi-
conductor material [11.1297] that is transparent to
dact
the laser emission (Fig. 11.104b). The resulting gain
Grating in active layer coupling in this grating structure is accompanied by
a strong index coupling due to the high refractive-
c) Grating layer: Eg < Eg, act index difference between the active layer and the re-
Ë
grown material. With respect to the phase difference
between the index and gain grating one distinguishes
between in-phase and anti-phase gratings.
• A current blocking pnp layer structure above the
dact active layer is corrugated and regrown, so that a pe-
Active layer: Eg, act
riodic variation of the current density injected into
Fig. 11.104a–c Various types of Bragg gratings. (a) Index the active layer is achieved [11.1298]. The parasitic
coupling; (b) gain coupling; (c) loss coupling index coupling can be kept very small in this type of
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 715

gain grating. Due to the Kramers–Kronig relations, the receiver. The photodetector retranslates the light
however, the gain grating is inevitably accompanied pulses back to the electronic bit sequence. Seen in terms
by an index grating. of a two-language dictionary, the laser translates ultra-
fast from electronics into optics and the photodetector
Loss coupling is obtained if the grating is etched into ultrafast from optics into electronics.
an additional layer that is separated from the active For this purpose, the electrons injected through
layer and is absorbing for the emission (Fig. 11.104c). the n contact in the semiconductor laser must arrive

Part C 11.3
This grating acts as a saturable periodic absorber for the as fast as possible at the most deeply bound energy
laser emission from the active layer [11.1299]. In con- states of the conduction-band QWs and the holes in-
trast to index coupling (Fig. 11.104a) the bandgap E g jected through the p contact as fast as possible into the
of the grating is smaller than the bandgap of the ac- ground states of the valence-band QWs (Fig. 11.105).
tive layer E g,act . Usually, the absorbing grating layer Several retarding physical transport and relaxation pro-
has a different refractive index than the material used cesses are involved, whose combined time delay effect
for the regrowth, so that considerable index coupling can however be minimized [11.1301, 1302]. Owing to
occurs. Alternatively, the loss grating can be integrated the very high doping in the long conduction paths,
into a metallization at the surface of the device, so that which start at the contacts, very short dielectric re-
no epitaxial regrowth is required [11.1300].
There are significant differences between the charac-
teristics of gain- and loss-coupled semiconductor lasers Laser emission
compared to index-coupled DFB lasers:
• In contrast to index-coupled devices, there is almost Blow-up
no reflection of the light wave in an ideal gain grat- p -doped
Injection bulk layer
ing. Thus, the interference of the reflected wave
current
inside the grating and at the facets is avoided, so
that the influence of the end facet phases is strongly
reduced compared with index-coupled DFB lasers. Contact
Therefore, a high single-mode yield can be obtained
without the necessity to use an antireflection coating
of the end facets. 1 0 0 1 0 1 1 0 ...
• The longitudinal photon distribution is, in the case Time t
of a small parasitic index coupling, similar to that of
an FP resonator. Thus, the strongly inhomogeneous Contact
photon distribution in DFB lasers and the result-
ing problem of longitudinal spatial hole burning is n-doped
bulk layer
reduced in gain-coupled devices.
y
Basics of Lasers
with High Modulation Bandwidth Bit pattern
For the highest-bit-rate fibre-optic data communication Light
(1.26–1.68 µm), the ultrafast conversion of the data 1 intensity
0
from the electronic bit sequence into the appropriate op- 0
1
tical bit pattern takes place by means of semiconductor 0
1
lasers. This is done either with a CW laser combined with 1
0.
a subsequent ultrafast optical modulator or via direct t ..
modulation of the laser (intensity or frequency modula-
tion). As the simplest example the intensity modulation Fig. 11.105 Schematic representation of the direct modula-
of the laser is described. The bit pattern available as a se- tion of a semiconductor laser, translation of an electronic
quence of ultrashort current pulses is translated by the bit pattern (left) via a corresponding temporal carrier dis-
laser into the appropriate sequence of ultrashort light tribution in the QWs (center) into an optical bit pattern
pulses, which then propagate e.g. via a fibre towards (bottom)
716 Part C Coherent and Incoherent Light Sources

In order to reduce optical losses through reabsorp-


tion, the confinement layers should be undoped or
Electrons (1) (2) (1) only slightly doped. Retarding effects arise as a con-
in the CB (5) (2) sequence of the charge-carrier transport (number 1 in
EC Fig. 11.106). Using the analogy of the balls and pipe
n-sided p-sided above, a ball in an empty pipe (undoped) must go
confinement (3) (4) confinement through the entire length of pipe (the length of a con-
layer (4) (3) layer
Part C 11.3

finement layer) before finally exiting from the other


end. Further retarding effects arise from the charge car-
(5) Holes rier capture (2), relaxation (3) in the respective QW
E (2) (1) in the VB
ground states, by the reconciliation of charge carrier
EV
inhomogeneities between the individual pots, through
y
tunneling (4) and thermal reemission (5). Since the mo-
Fig. 11.106 Schematic representation of the charge carrier dynamics bility of the electrons is substantially higher than that
close of the active region (here seven QWs) in the band structure in of the holes, in asymmetrical laser structures [11.1302]
space for an asymmetric laser structure [11.1302] (enlargement of the p-side confinement layers are reduced in thickness
Fig. 11.105 in the area indicated by the ellipse) in favor of the n side. This favors the transfer of the
less-mobile holes. In addition, this asymmetric laser
laxation times arise there. This can be visualized by structure design takes into account the different cap-
means of a pipe completely filled with ping pong balls ture probabilities: the capture of holes into the QWs
(high doping throughout the length of the conduction is much more efficient than that of electrons. Thus,
path). A ball injected at one end of the pipe, causes an- a smaller p-sided confinement layer (reservoir of uncap-
other to be ejected from the other end of the pipe. In tured electrons giving rise to bit interfering) is beneficial.
this manner, a current pulse is transferred to the other In today’s fastest laser diodes (largest modulation band-
end of the pipe almost without delay in heavily doped width) −3 dB modulation frequencies of up to 40 GHz
semiconductors. can be obtained.

a) d)
GAC
WG 1
WG 2
DFB

b) e)

DBR SG

c) f)
GCSR
WG 2
WG 1
TTG

Fig. 11.107a–f Schematic cross-sectional views in the y–z-plane of different laser types: (a) three-section DFB, (b) three-
section DBR, (c) TTG, (d) GAC, (e) SG, which is related to the SSG laser (not displayed) and (f) GCSR
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 717

a) b) w
J (z) DFB grating
Ëz
z

x
bent

Part C 11.3
waveguide
x (z) w

IB TiPtAu SiO2
d) Au

IC
z
p-InGaAs
Au x
s.i.-InP
Is c)
1.21µm InAlGaAs IS IC IB IB IC IS
Au
InGaAs/InAlGaAs
multiple QW
SiO2 active region
Chirped DFB Chirped DFB
1.21µm InAlGaAs
p-InP y
n-InP substrate

AuGe w

Fig. 11.108a–d Schematic perspective view of (a) a Y-laser [11.1303] and (b-d) three-section bent-waveguide chirped
DFB lasers [11.1304], (b) the principle of generating chirped DFB gratings by specifically bent waveguides on homoge-
neous grating fields, cross section of two independent lasers originating from the bending displayed in (b), (d) perspective
schematic of a device shown in (c). A scanning electron micrograph (SEM) of such a tunable three-section chirped DFB
laser is displayed in Fig. 11.116a

Tunable Lasers (center) [11.1308]. The phase section only includes the
Wavelength tuning of an edge-emitting DFB semicon- brown waveguide layer(s) and is used to match the
ductor laser can be obtained according to (11.93), in phase of the standing light wave after one round-trip.
the simplest case, by varying the effective refractive in- The gain is controlled, e.g., via the current between
dex via the injection currents in different sections, either the top right contact and the bottom contact. In con-
thermally or by using plasma effects (carrier density trast, a vertical separation is used in the tunable twin
variations). In these cases rising injection currents lead guide (TTG) laser [11.1306, 1307, 1309] (Fig. 11.107c).
A current from the left-side contact to the top contact
1. to increasing emission wavelengths (red shift) via only controls the carrier density in the brown waveguid-
thermal effects and ing layer. The gain is controlled via the current between
2. to a blue shift via the plasma effect. the left side contact and the bottom contact. In the three-
section DBR and the TTG laser the tuning is based on
A superposition of both effects is found in multi-section the plasma effect, if only forward biasing is used.
DFB lasers [11.1305] since gain, tuning and DFB grating Another very important tuning principle is based on
exist in all sections (Fig. 11.107a). In order to increase two mode combs of slightly different mode spacing. In
the total tuning range it is necessary to separate gain analogy to a vernier based on two scales [11.1306,1307],
and tuning [11.1306, 1307]. In the three-section DBR a small detuning of the combs can address individual
laser (Fig. 11.107b) this is done longitudinally by us- modes separated widely in the spectrum: only those
ing a gain section (right, the active region is shown modes which exactly occur in both combs can oscillate
in black), a grating-section (left) and a phase section since only this situation provides sufficient reflectivity
718 Part C Coherent and Incoherent Light Sources

Table 11.37 Tuning characteristics of different 1.55 µm laser types, DFB: distributed feedback, DBR: distributed Bragg reflector,
TTG: tunable twin guide, SSG: superstructure grating, SG: sampled grating, GAC: grating-assisted coupler, GCSR: grating-
assisted co-directional coupler laser with rear sampled grating reflector. The tuning occurs either thermally (t), via the plasma
effect (p), via the co-directional coupler (CC) grating or via Vernier effect (V). TR: tuning range
Laser type Control Tuning Tuning Tuning Miscellaneous Ref.
currents (exp.) (max. con- principles
Part C 11.3

(∆λ/nm) tinuous)
3 sect. DFB 2 3 3 t, p Continuous TR [11.1305]
3 sect. DFB 2 5.5 3 t, p Bent waveguide, quasi contiunuous TR [11.1294, 1304,
1312]
3 sect. DBR 3 10 7 p, (t) Quasi continuous TR [11.1313]
3 sect. DBR 3 22 7 p, t Incl. both polarities, quasi continuous TR [11.1314]
3 sect. DBR 3 7 p Mode-hop-free, really continuous TR [11.1315]
TTG 2 7 13 p, (t) Continuous TR [11.1306, 1309]
TTG 2 13 13 p, t Incl. both polarities, continuous TR [11.1306]
Y 4 51 V, p No continuous TR [11.1303]
SSG/SG 4 95 V, p Quasi contiunuous TR, gaps in the total TR [11.1310, 1311]
SSG/SG 11 38-50 V, p Quasi contiunuous TR, [11.1316]
without gaps in the total TR
GAC 3 50-70 CC, p No continuous TR [11.1262, 1317,
1318]
GCSR 4 100 CC, p Quasi continuous TR, [11.1319]
without gaps in the total TR
GCSR 4 50-114 CC, p Quasi contiunuous TR, gaps in the total TR [11.1320]
SSG/SG TTG 3 30-50 V, p Quasi contiunuous TR [11.1321]
MG-Y 4-5 46 V, p Quasi contiunuous TR [11.1322]

and, thus, sufficient net gain. This principle is applied different tunable laser types with respect to important
in the (C3 ) laser, Y laser, Mach–Zehnder interferome- device characteristics and properties.
ter laser, superstructure grating (SSG) DBR laser and Generally the types discussed up to now cannot
sampled grating (SG) laser. Two FP cavities of differ- provide excellent characteristics in all features such
ent length and, thus, two FP mode combs are used in the as simple tuning (low number of control parameters),
Y laser (Fig. 11.108a) and the C3 laser (two coupled FP high SMSR, wide tuning, continuous tuning and high
lasers of slightly different length, not displayed). Two su- efficiency. This motivates the search for promising com-
perstructure mode combs are shifted against each other binations of the above principles. Using a GAC to select
in the SSG laser [11.1310] and SG DBR laser [11.1311] a mode from an SG yields the grating-assisted codirec-
(Fig. 11.107e). The codirectional coupling in the grating tional coupler laser with rear sampled grating reflector
assisted coupler (GAC) laser between two waveguides (GCSR) [11.1319, 1320] (Fig. 11.107f). Another laser
realizes an additional spectral filter which can be shifted with 11 sections combines a SSG or a SG with many
spectrally in a controlled way against an FP mode spec- DBR sections of different grating period each [11.1316].
trum. The two waveguides can be laterally or vertically SSG or the SG laser and the TTG laser has been pro-
(Fig. 11.107d) coupled. Depending on the size of the posed [11.1321]. Combining the SSG laser and the Y
grating period, a grating can reflect light (inversion of laser yields the modulated grating Y laser [11.1322].
the propagation wave vector, contra-directional coupling For comprehensive details of tunable lasers we refer
grating, short grating period, e.g., Fig. 11.107a,b,c,e) or to [11.1306, 1307]. Finally, coupled Mach–Zehnder in-
change the magnitude of the propagation vector (main- terferometers or arrayed waveguide (AWG) structures
taining propagation direction, codirectional coupling can also be used as filter structures in lasers, e.g., in
grating, long period, shown in Fig. 11.107d below the the digitally tunable ring laser using a ladder of ring-
center contact). Table 11.37 includes a comparison of resonator filters [11.1323, 1324].
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 719

DFB lasers with an axially varying grating period


2.1
are very attractive to tailor specific device properties. 1.0 1.0
1.0 Conduction band
4.7
Using bent waveguides on homogeneous DFB gratings 1.5nm
(Λz = const.) enables to generate a local effective pitch Electron
3
length Λ(z) that exceeds Λz the more, the larger the ù
local tilt angle of the bent waveguide deviates from AlInAs barriers
6.1 2 3
a vertical intersection of the pitches i. e., the larger 4.5 1
4.0 3.8 ù

Part C 11.3
Photon emission
the local tilt angle ϑ(z) is. Figure 11.108b schemati- 3.4
8.2 nm 2
cally shows a bent waveguide covering a homogeneous 1 Electron
grating. Choosing appropriate bending functions x(z) GaInAs QWs
generates chirped DFB gratings with a varying effective Laser- Electron Laser Electron Laser-
active injection active injection active
pitch length Λ(z) = Λz / cos(ϑ(z)), as shown in the inset
to Fig. 11.108b [11.1294]. The fabrication method is in- Fig. 11.109 Principle of a quantum cascade laser [11.1326]
dicated in Fig. 11.108c, which shows two chirped DFB
lasers formed after cleaving the structure in Fig. 11.108b Through tailored dimensioning, we ensure that in
in the x-direction in the center of the side of the device the case of resonance (for a certain applied voltage)
oriented in the z-direction. Since the light is strongly each of the four narrowest QWs exhibits a bound state,
guided along the bent w-direction, the light sequen- and that these four states are energetically identical
tially passes quasi continuously varying pitch lengths (i. e., they line up exactly horizontally). Furthermore,
Λ(w), as displayed in Fig. 11.108c. Since ϑ is largest the widest QW is dimensioned in such a way that the
in the center of Fig. 11.108b, the two chirped DFB highest state of the three bound states, marked with
lasers have the largest pitch at the center facets. Var- a 3 in Fig. 11.109, deviates only insignificantly from
ious applications of chirped DFB gratings have been the four identical levels mentioned above. Due to the
demonstrated [11.1294,1304,1312,1325], including ax- thin barriers and the resulting tunneling processes, an
ially distributed phase shifts, higher SMSR, enhanced electron injected from the left tunnels horizontally into
single-mode stability and lower line widths. In addition, the excited level 3. After a radiative transition it falls
chirped three-section DFB lasers (Fig. 11.108d) have down to level 2. Due to the very thin barriers, the wave
demonstrated enhanced tuning ranges [11.1294, 1304, functions are generally strongly delocalized. By opti-
1325] (Table 11.37). The mushroom-type laser struc- mizing the QW geometries the relaxation time from
ture (Fig. 11.100d) is applied in the chirped three-section state 2 to state 1 is designed to be very small, so that
DFB laser (Fig. 11.108d), which shows a modulation the maxima of the wave function of state 2 lies on
bandwidth of up to 26 GHz [11.1302]. the left and that of state 1 on the right of both of the
wider QWs.
Further Laser Types with Horizontal Resonators This tunneling process proceeds in a stair-like cas-
In the bipolar lasers considered so far the light emission cade, which is illustrated with just two stages in
in the active layer takes place through the recombina- Fig. 11.109. This example also illustrates very success-
tion of an electron in the conduction band with a hole in ful recent complex QW structures, which are based on
the valence band (band–band transition or inter-band a variety of different quantum cascade structures. Quan-
transition). In unipolar lasers the radiative recombi- tum cascade lasers are very successful to produce laser
nation takes place within a single band between two emissions in the mid infrared (3.5–10 µm, in some cases
bound states of a potential well (intra-band transition, even up to 60 µm), where there are very few suitable
in Fig. 11.109 shown for the conduction band). Through semiconductor materials with extremely small bandgaps
so-called electron recycling, this process is cascaded for the construction of bipolar lasers.
in stages (explaining the name quantum cascade laser, A very elegant way to obtain a longitudinal single-
Fig. 11.109). The band edges are accordingly tilted by mode oscillation of an FP laser is to use one highly
the applied voltage (electric field). The multiple-QW reflecting (HR) and one antireflection (AR) coated facet,
structure [11.1326] shown here is based on a uniform with a piece of fibre optically coupled to the latter
QW composition and a different uniform barrier com- (Fig. 11.110a) including a DBR grating with a period
position. However, there are in each case six different ((11.93)) such that it filters exactly one single oscillat-
QW widths (the lower sequence of numbers) and barrier ing mode from the spectral amplification profile. This
widths (the upper sequence of numbers) involved. laser design is called a (semiconductor-)fibre laser. In
720 Part C Coherent and Incoherent Light Sources

the beginning and end of the resonator merge into one


a) Laser active region DBR grating in fiber core another. In the case of waveguiding (Fig. 11.110b) modal
solutions result if the length of the circular optical axis
HR AR
is close to an integer multiple of the wavelength in
the medium. Similar selection rules apply in micro-
disc lasers, which can also be illustrated in the ray
Fiber cladding Fiber core model with multiple reflections (eight in Fig. 11.110d)
Part C 11.3

at the exterior surfaces. These modes are also known as


Resonator whispering-gallery modes after the acoustic phenomena
in the gallery of the St. Paul’s cathedral in London and
b) the Gol Gumgaz mausoleum in Bijapur city in India.
There, a whispered word is discernible, after multiple
reflections from the inner walls of the cupola, back at
the ear of the speaker.

11.3.4 Basics of Surface-Emitting Lasers


with Vertical Resonators (VCSELs)

c) The VCSEL presents a large technological challenge in


terms of the implementation of DBR mirrors with ex-
Circular tremely high reflectivity. In contrast to the edge-emitting
waveguide DFB or DBR laser, the individual layers of the DBR
mirrors in the VCSEL are successively deposited (e.g.,
Straight
by epitaxy). In this way, layer A and the neighboring
waveguide Coupling layer B together make up one period. Since the reflec-
tivity of the DBR mirrors rises with increasing number
of periods and refractive index contrast, materials with
large refractive index contrast are preferable in order
to reduce the total number of periods and thus device
d) cost. The insets in Fig. 11.111 show a DBR mirror (left
inset) and the light intensity reflected by the mirror
as a function of the wavelength (reflection spectrum,
right inset). For λ = 1.55 µm, the maximum reflectiv-
ity Rmax in the stop-band is presented in the main
picture as a function of the number of periods for dif-
ferent material systems. The data result from theoretical
model calculations with consideration of the spectral
variations of the refractive indices and absorption coef-
ficients [11.1328, 1329]. Large differences appear in the
Fig. 11.110a–d Various designs of lasers with horizon- figure due to different absorption and different refractive
tal resonator. (a) FP laser with an external fibre mirror, index contrast 2(n A − n B )/(n A + n B ). For semiconduc-
(b) double ring resonators coupled to a straight waveguide, tor epitaxial layers, absorption depends on the doping
(c) standing wave in a single ring resonator coupled to 2 concentration and is well controllable. Absorption in di-
waveguides, (d) DFB microdisc laser [11.1327]; inset: FP electric layers is more difficult to control and depends
microdisc laser with whispering-gallery mode strongly on the technological process. Unfortunately, no
large refractive index contrasts can be realized in the
contrast, the active medium for optically pumped fibre GaInAsP material system. To achieve a reflectivity of
lasers is a doped fibre. 99.8%, 50 periods, a number that is in practice too high,
Laser designs with straight aligned resonators have are needed. In contrast, this is achieved in AlAs/GaAs
been considered so far. However, in the ring laser DBRs with just 20 periods. If the two dielectrics Si3 N4
(Fig. 11.110b, c) and the microdisk laser (Fig. 11.110d), and SiO2 are combined, then even 13 periods are suf-
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 721

ficient due to the very high relative refractive index


contrast. Maximum spectral reflectance Rmax
This enormously high reflectivity is achieved ë = 1550 nm
through constructive interference of the partial waves Rmax
reflected at all heterointerfaces. Note that with a reflec-
tion at the interfaces from the optically thinner to the
á = 0 cm-1
optically denser medium a phase change of π occurs, 0.99999 á = 0.1 cm-1

Part C 11.3
but not vice versa [11.1330, 1331]. The condition for
InP/air gap
constructive interference is fulfilled, e.g., by the com- 0.9999 DBR mirror á = 1 cm-1
bination of λ/4-thick layers A and B, as is the case
in Fig. 11.111. Here, dA and dB are the physical thick- 0.999 á = 10 cm-1
nesses and λ/4n A and λ/4n B are the optical thicknesses. á = 20 cm-1
0.99 á = 100 cm-1
In general, the following relation applies to achieve high
SiO2 / Si3N4
reflectivity using constructive interference DBR mirror
0.9 AlAs/GaAs
λ DBR mirror
n A dA + n B dA = m (with m = 1, 3, 5 . . . ) . 0.5
2 0 5 10 15 20 25
(11.120) Number of periods

On GaAs substrates the almost lattice-matched Fig. 11.111 Maximum spectral reflectivity Rmax in the stop-band for
AlAs/(Al)GaAs combination is ideal for lasers in the λ = 1.55 µm as a function of the number of periods for different
wavelength range 800–1300 nm. Although, as with DBR mirror systems. Left inset: cross section of a DBR mirror.
the edge emitters, trials have been made to imple- Right inset: reflectivity as a function of wavelength
ment long-wavelength VCSELs on GaAs substrates,
1.55 µm VCSELs are still based on InP. This is due the electrons are injected from below through the lower
to the fact that the active laser layers (e.g., GaInAsP n-doped DBR mirror. The outer curved black arrows in-
and AlGaInAs) for the spectral range close to 1.55 µm dicate the current flow. Here, it is challenging to reduce
can be best implemented on InP substrates. There are the electrical resistance of the p-doped DBR mirror by
different possibilities for implementing highly reflect- sophisticated doping (impurity concentration profiles) in
ing 1.55 µm DBR mirrors on InP substrates: a kind of order to reduce the operating voltages and the buildup of
pressure bonding technique (wafer fusion) of Joule heating. Figure 11.112a schematically depicts the
AlAs/GaAs DBRs [11.1332, 1333] to embed the structure of a VCSEL with two dielectric DBR mirrors.
GaInAsP active region, strongly lattice-mismatched so- The holes and electrons are injected by means of ring
called pseudomorphic AlAs/GaAs DBRs [11.1334], contacts, whereby the current flow bypasses the elec-
lattice-matched AlGaInAs, AlAsSb/AlGaAsSb, trically insulating DBR mirrors. Furthermore, of crucial
AlGaAsSb/InP DBRs [11.1335, 1336] or fusing of importance is the lateral electrical confinement to enable
a low-period GaInAsP/InP DBR with active layers onto the production of high electron–hole-pair densities in the
a AlAs/GaAs DBR [11.1337]. central part of the active zone, and thereby very small
A resonator results from the combination of two threshold current densities. Therefore, an electrically in-
DBR mirrors, where the volume between the DBR sulating ring is built surrounding the lateral laser mode.
mirror-ends towards the center is called the cavity. If The realization of this is technologically demanding and
the cavity material is passive, then the setup is an optical is achieved, e.g., by ion implantation or selective oxi-
filter, if it is active then a VCSEL results. Figure 11.112 dation. A sufficiently high thermal conductivity of the
shows schematically the structure of a VCSEL with two DBR mirrors is of further importance in enabling effi-
multiple-layer semiconductor DBR mirrors. In the illus- cient heat dissipation from the active region to the heat
tration the upper mirror is highly reflective, so the laser sink and, if necessary, of that heat generated inside the
light is emitted essentially downwards (brown arrow). DBR mirrors.
The envelope of the vertical intensity distribution dis- For the VCSEL with two dielectric DBR mirrors
cussed below is indicated by the lateral expansion of and a cavity length of 3λ/2 shown in Fig. 11.112a,
the brown arrow (Fig. 11.96, depicted in grey-tone vari- the electric field of the standing light wave is com-
ations). The holes are injected from above through the puted [11.1328, 1329] and presented in Fig. 11.113
upper p-doped DBR mirror into the active laser zone; together with the entire multilayer structure. In order
722 Part C Coherent and Incoherent Light Sources

a)
p contact SiO2

DBR2 Si3N4

Laser-active GaInAsP
layer ë
3
2 GaInAs QWs
Part C 11.3

cavity
DBR1
n substrate
Standing wave
n contact (electric field)

Fig. 11.113 Layered structure of a VCSEL including the


b) standing wave of the electrical field
p contact

for higher mirror reflectivities. This means that a cavity


DBR2
of this length is suitable for each of these (laser) wave-
lengths if the standing wave experiences a sufficiently
large optical gain at its peak (antinodes). On the con-
Laser-active trary case, for a desired (fixed) laser wavelength λ the
layer
cavity length can be selected straight away as λ/2, 2λ/2
or 3λ/2. If the two mirrors are implement as DBRs (bot-
DBR1
tom left of the figure), then the line spectrum at the top
right is superposed with the known reflection spectrum
n substrate (Fig. 11.114 bottom right) of the DBR mirrors, resulting
n contact in the laser spectrum already shown in Fig. 11.103d. The
stop-band of the VCSEL is substantially larger because
of the higher refractive index contrast in the DBR mir-
rors compared to that of the DFB laser with the relatively
Fig. 11.112a,b Schematic setup of a VCSEL with elec- small refractive index contrast between the quasi-layers
trically insulating (a) and electrically conducting DBR of the DFB grating. Following from Fig. 11.103c, d the
mirrors (b) λ/4-phase-shifted DFB laser has many similarities to
a VCSEL with a λ/2 cavity and two very long DBR
to achieve a high gain in the laser design, the QWs are mirrors with a small refractive index contrast.
positioned at the maxima (antinodes) of the half-waves. Note that the following numerical values are strongly
Ideally, three QWs, three double QWs or three triple dependent on wavelength and material and that a thor-
QWs should be placed in the 3λ/2 cavity shown. The oughly comprehensive treatment would exceed the
envelope of the standing light wave field gradually drops framework of this volume. For VCSELs, optical power
outwards from center due to the distributed reflecting ef- outputs of < 1 mW (lateral single-mode operation) are
fect of the DBR mirrors. We note again that exactly one typical. With a laterally expanded active region, i. e.,
quarter of a wavelength is allotted to each mirror layer laterally multimode VCSELs, achieve up to 120 mW.
(λ/4 layers) and that the nodes for the design wavelength Typical threshold currents lie around 1 mA, with record
lie exactly at the interfaces. values of about 0.06 mA (corresponding to 350 A/cm2 ).
In the following, the VCSEL spectra are intuitively The highest power outputs and the lowest thresholds
constructed. To derive this, we consider a semiconduc- are achieved in the spectral range 850–1000 nm. Com-
tor cavity between two mirrors indicated in the top left pared to edge emitters the thresholds are amazingly
of Fig. 11.114. Based on the fixed cavity length, (11.92) low, but with rather moderate maximum power out-
leads to the three modes displayed as lines in the spec- puts. In broad-area edge emitters for example, over
trum on the right of the figure, which become sharper 6 W [11.1338] and external quantum efficiencies of
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 723

over 56% [11.1338] have been achieved. While the


Semiconductor
VCSEL has enormous advantages in the laser–fiber Mirror 2 cavity
coupling due to the small beam divergence and the b c c b a
a
symmetric mode profile, the edge emitter incurs sub-
stantial overhead costs for light coupling due to the
higher divergence and the elliptical mode profile. This Mirror 1 Selection of cavity modes
is achieved in practice with aspherical lenses or with

Part C 11.3
complicated tapered waveguide structures in the laser
1 1.5 2 2.5
or fibre. The VCSEL offers further substantial ad- ëair (µm)
vantages as it enables simple optical on-wafer testing DBR 2
similar to the testing of integrated electronic circuits. QW3
In contrary, edge emitters must be individually iso- QW2
lated for characterization, i. e., at least cleaved into bars, QW1
or additionally for surface out-coupling, a 45◦ mirror DBR 1
Reflection spectrum
(Fig. 11.96) must be implement in combination with
of a DBR mirror
etched mirrors.
The modulation bandwidths of VCSELs are typ- Fig. 11.114 Characteristic spectral components of a VC resonator.
ically around 1 GHz (the record being 10 GHz), Three standing waves in the cavity ((a–c) above left) cause, as
compared with typical values of 15 GHz (the record marked by the bracket, the build up of the FP modes (above right),
being 40 GHz) for edge emitters. If one compares the the DBR mirrors (bottom left) are characterized by the reflection
laser line widths of devices without external resonators, spectrum (bottom right), as indicated by the two brackets. With
then VCSELs typically attain 200 MHz (the record be- a very short cavity length only one FP mode is located in the stop
ing 50 MHz) while edge emitters typically attain 1 MHz band (along the broken vertical lines)
(the record being 10 kHz). Edge-emitting semiconduc-
tor lasers exist in the range between 350 nm and 12 µm, For λD in a DBR mirror, all reflected partial waves in-
while in the green and mid-IR spectral regions there are terfere constructively (99.9% reflection) on the incident
as yet either no devices exist or the component lifetimes side of the mirror and destructively on the opposite side.
are not sufficient for practical applications. Electrically This is the result of complicated multiple reflections and
pumped VCSELs exist so far within a spectrally much complex zigzag paths (in the simple ray model) por-
smaller range (420 nm to 2.05 µm) [11.1339–1341]. In trayed in a simplified manner occur. The light waves
VCSELs wavelength tuning is particularly difficult us- penetrate the mirror, but due to the perfect destruc-
ing charge-carrier-induced (current-induced) or thermal tive interference, behind the mirrors, they transfer no
refractive index changes. A typical tuning range of 1 nm energy. By the targeted positioning of the second mir-
is attained in VCSELs compared to 80 nm in single- ror (and adding further boundary surfaces) all partial
mode edge emitters. Finally we present a tuning concept waves now interfere destructively on the incident side
for optoelectronic devices with vertical resonators which and constructively on the opposite side (behind the sec-
permits ultrawide wavelength tuning on the basis of only ond DBR mirror). Furthermore, a standing wave forms
one control parameter. in the cavity for λD (Fig. 11.114).
Within the stop-band, except within the range of the
Micromechanical Tunable Filters and VCSELs very sharp filter line (centered at λD ) all wavelengths
A perpendicular light wave (wavelength λD ) incident on are up to 99.9% reflected. In this way extremely high-
a highly reflecting DBR mirror is up to 99.9% reflected. quality optical filters can be implement, e.g., for fibre-
The period is normally selected in such a way that λD lies optic telecommunications based on dense wavelength
at the center of the stop-band (Fig. 11.114 bottom right). division multiplexing.
When a second identical mirror is positioned parallel at Figure 11.111 contains a further material system,
a distance, say, 1.5 × λD from the first one, as shown in so far not discussed, with an extremely high refractive
Fig. 11.114, it is experimentally observed that the first index contrast (n InP = 3.2, n air = 1). With only four pe-
mirror does not reflect the wavelength λD any more. riods, a reflectivity of over 99.8% can be obtained. This
Although at first sight astonishing, the arrangement of unusual structure can be made, e.g., from a semicon-
the two DBR mirrors is now almost 100% transparent ductor multilayered structure with alternating InP and
for λD . Ga0.43 In0.57 As layers by selective etching of the GaInAs
724 Part C Coherent and Incoherent Light Sources

a) c) Wavelength tuning (nm)


Suspension
0

Membrane
–20

–40
Part C 11.3

Supporting
post
–60

1400 1500 1600


–80
b)
DBR 1 –100
2.5 periods
GaInAsP/air
–120
ë/2 air cavity

DBR 2 –140
2.5 periods
GaInAsP/air 1400 1500 1600

InP substrate –160


0 –0.5 –1 –1.5 –2 –2.5 –3 –3.5
Actuation voltage (V)

Fig. 11.115a–c Micromachined filter device with vertical resonator based on semiconductor multiple air gaps [11.1342,
1343]. Electron micrograph of the cross section of a filter (a), details in (b), corresponding experimental wavelength
tuning as function of the actuation voltage in (c)

layers (micromechanical sacrificial-layer technology). (Fig. 11.116a,b) and quantum photonics (Fig. 11.116c,d)
Lattice-matching already exists through epitaxy on an can be drawn. In order to tailor the electronic levels
InP substrate and, if necessary, an outstanding com- for electrons and holes, semiconductor heterostructures
patibility with 1.55 µm GaInAsP laser-active layers of predetermined composition and thickness are imple-
is available. Figures 11.115a,b show a filter structure mented. If the layer thickness of the material with the
with six InP membranes, each of which is fixed to smaller bandgap is on the order of the magnitude of the
the supporting posts at four points. If a reverse-bias electron wavelength, a quantization occurs that leads to
voltage is applied between the upper p-doped and the defined quantized energy levels in the QWs. These quan-
lower n-doped DBR mirrors the membranes includ- tized energy levels (eigenvalues) and the corresponding
ing the sandwiched air cavity can be electrostatically electronic wave functions (eigenfunctions, i. e., modes)
actuated. The cavity length and thus the filter wave- are solutions of the Schrödinger equation. The materials,
length can be varied in this way with only one control stress and layer thicknesses are set up in this example
parameter (voltage). With such an optical filter, an enor- with the 10 AlGaInAs QWs (Fig. 11.116b) in such a way
mous continuous wavelength tuning range of 142 nm that the optical emission is at 1.55 µm. These QWs serve
(Fig. 11.115c) was experimentally achieved with only as the laser-active medium of an ultrafast semiconductor
3.2 V [11.1328, 1329, 1342, 1343]. In other structures of diode laser (Fig. 11.116a) [11.1302,1344]. In a very sim-
the same type, a continuous tuning range of as much as plified depiction, the multiple QWs define a resonator
221 nm has been obtained [11.1342]. The same tuning for electron waves.
principle occurs in Figures 11.116c,d showing a VCSEL The electron microscope micrographs on the right
with InP/multiple-air-gap DBR mirrors, GaInAsP laser- show the exact analogy for photons. In order to select
active QW layers and an InP substrate. a defined mode in the resonator of a VCSEL, taking
In conclusion, based on Fig. 11.116 a very into account the refractive indices, layer thicknesses
interesting parallel between quantum electronics in the order of magnitude of the photon wavelength
Lasers and Coherent Light Sources 11.3 Semiconductor Lasers 725

are chosen. A kind of quantization also arises in this


case. The effective refractive indices (eigenvalues) and 1.55 µm DFB edge emitter 1.55 µm VCSEL
the corresponding photon wave functions (eigenfunc- a) b)
tions, i. e., modes) are solutions of the Helmholtz
equation. From the mathematical point of view, the
space-dependent parts of the Schrödinger and Helmholtz
equations have equivalent behavior. The strong re-

Part C 11.3
100 µm
fractive index contrast of InP/air-gap multi-membrane
structures is again used in Fig. 11.116d to implement
highly reflective DBR mirrors for a 1.55 µm VCSEL
(Fig. 11.116c) [11.1342, 1343]. Analogously the peri-
odic refractive index variation defines a resonator for
photon waves.
Further analogies in this area are offered by
periodic 2-D quantum-dot fields and 2-D photonic crys-
tals, or photonic band structures and electronic band 100 nm 3 µm
c) d)
structures.
AlGaInAs/AlGaInAs MQWs GaInAsP/air-gap DBR
electron wave resonator lightwave resonator
11.3.5 Edge-Emitting Lasers and VCSELs
with Low-Dimensional Active Fig. 11.116 (a) Tunable, edge-emitting three-section laser with
Regions axially varying DFB grating known as a chirped DFB grat-
ing [11.1294], (b) strain-compensated multiple QW structure with
In commercial semiconductor laser diodes, bulk semi- tensile-strained AlGaInAs barriers and compressively strained
conductor materials (3-D) were exclusively used for AlGaInAs wells[11.1344], (c) VCSEL based on multiple InP/air
the active zones for 25 years. Starting from 1990 edge membranes (centre), each of which is supported by four suspensions
emitters with QWs (2-D) were implement in research connected to the square supporting posts [11.1343], (d) cross sec-
labs and continuously improved. Only after a further tion of the vertical resonator, consisting of the laser-active GaInAsP
five years QW lasers were commercialized and subse- QW region, which is embedded between two InP/air-gap DBR
quently surpassed the 3-D lasers with lower threshold mirrors [11.1342]
current densities, higher power outputs, higher char-
acteristic temperatures T0 and higher bit rates due to development effort is expected to provide excellent
more-favorable gain profiles and better electronic con- QD lasers.
finement. Although quantum wire (1-D) lasers should
exhibit even better characteristics, they have so far not 11.3.6 Lasers with External Resonators
been very successful due to technological and geo-
metrical constraints. In particular long carrier-transport Both edge emitters and VCSELs can be implemented, as
and carrier-capture times substantially limit the bit shown in Fig. 11.96, with an external resonator mirror,
rates in quantum wire lasers. Quantum dot QD (0- in contrast to Figs. 11.115 and 11.116c, which involve
D) laser structures [11.1263–1272] are a lot more a relatively large air gap. This can serve several purposes:
promising. However, a problem at the moment is the
strongly varying size of QDs (Fig. 11.93). The theoret- 1. the extension of the resonator length to achieve
ically very sharp density-of-state profiles are strongly narrower line widths,
inhomogeneously spread, so that the predicted high 2. wavelength tuning by inserting a wavelength-
differential gain dg/ dn does not arise in practice. selective, rotating element (prism, etalon, grating),
Compared with the 3-D and 2-D structures so far no 3. mode coupling for the generation of periodic se-
spectrally narrower and higher-gain profile has been quences of ultrashort pulses and
obtained. Particularly broad gain profiles can be of ad- 4. wavelength conversion by insertion of an optically
vantage however for extremely widely tunable lasers nonlinear crystal.
(see the section on tunable lasers in Sect. 11.3.3 and that
on micromechanical tunable VCSELs in Sect. 11.3.4). Examples of the last of these are lasers in which
However, as already mentioned, additional research and a frequency-doubling crystal in the air gap of the res-
726 Part C Coherent and Incoherent Light Sources

onator transforms the IR light, which is emitted from an cavity VCSEL (active region plus one DBR mirror), into
edge emitter with one side antireflection-coated or a half- the yellow, green and blue range.

11.4 The CO2 Laser


Part C 11.4

The CO2 laser is one of the most important lasers sion wavelength of 10.6 µm, special tunable CO2 lasers
for industrial, medical and scientific applications. Ap- can generate laser light at dozens of distinct emission
plications include high-precision material processing, lines between roughly 9.2 µm and 11 µm. Such lasers
cutting and welding of sheet metal, marking of plas- are used for scientific applications such as molecular
tics, cutting of paper and fabrics, surface treatments for spectroscopy and optically pumping of far-infrared gas
steel hardening or medical applications such as tissue lasers.
coagulation. The physical principles and the technical realizations
CO2 lasers use a gas mixture of helium, nitro- of typical CO2 lasers are described in the following
gen and carbon dioxide as the active medium, which sections.
is usually excited by an electrical gas discharge. The
key characteristics are emission in the mid-infrared 11.4.1 Physical Principles
at wavelengths around 10 µm and a continuous-wave
output power ranging from a few watts for sealed-off Basic CO2 Laser Tube Principles
miniature laser modules to more than 10 kW for high- Laser action in a CO2 gas was first described by Patel
power CO2 lasers with fast gas flow. While most CO2 in 1964 [11.1345, 1346]. The basic physical principles
lasers operate in a CW mode with quite fast power have changed little since then. An excellent and de-
modulation enabled by electrical excitation, there are tailed discussion of CO2 laser fundamentals is given
also pulsed systems based on Q-switching or the so- in [11.1347] while additional general laser fundamentals
called tranversal-excited atmospheric-pressure (TEA) are described in [11.1348] and [11.1349]. Figure 11.117
laser. The beam quality is often excellent and in many shows a sketch of a basic longitudinally direct current
cases nearly diffraction-limited. This is important for ap- (DC)-excited CO2 laser. The laser gas is usually a mix-
plications such as precision cutting or remote welding. ture of CO2 , N2 and He in a ratio of 1:2:8, for example.
The mid-infrared emission implies that standard glass The total gas pressure in such a DC-excited laser is
lenses and glass fiber-optic waveguides cannot be used a few tens of hPa. The gas is excited by an electrical
because of the high infrared absorption of silica-based gas discharge, for example by a steady longitudinal DC
glasses. Transmitting optics such as focussing lenses glow discharge inside a quartz glass tube. Typical re-
or partially reflecting mirror substrates are commonly quired voltages are 15 kV per meter of discharge length,
made of zinc selenide, silicon or germanium. For beam with a DC current of a few tens of mA. The voltages
guidance moving-mirror systems mounted on linear and needed to start the discharge can be considerably higher.
swivel axes are used. Besides the most common emis- To maintain a stable α-type glow discharge [11.1350]

Rb + –
A UDC K Brewster window

Beam
Laser gas

Plane total reflector Sperical


Cooling jacket
output coupler
Water coolant

Fig. 11.117 Basic longitudinally DC-excited CO2 laser


Lasers and Coherent Light Sources 11.4 The CO2 Laser 727

an external ballast resistor Rb is required in series with a high thermal population of the lower laser energy lev-
the high-voltage power supply. This compensates for the els, the CO2 laser gas must be kept cool at temperatures
differential negative impedance characteristic of the gas of 400–500 K, depending largely on the different CO2
discharge and limits the discharge current in order to laser types. A simple method for cooling is a second
prevent arcing. Alternatively, power supplies with fast glass tube, which acts as a cooling jacket coaxial to the
voltage- and current-regulating electronics can be used. laser gas tube with a continuous water flow, as shown in
Typical lengths of the gas discharge are on the order of Fig. 11.117.

Part C 11.4
one meter, depending on the desired output power. A rough estimate for these diffusion-cooled DC ex-
Such laser tubes can be filled once with the laser cited lasers is an output power per discharge length of
gas mixture and are then sealed-off for the lifetime of 80 W/m. This cannot be scaled by using larger cross
the laser tube. Other lasers are provided with a gas in- sections of the laser tube since this would reduce the
let and outlet to maintain a gas flow through the laser amount of thermal energy that can be removed from the
tube. This improves the laser power as fresh laser gas is middle of the gas discharge by diffusion cooling to the
provided to the laser but also requires additional periph- walls. The overheating of the gas and the resulting ther-
erals such as gas reservoirs and vacuum pumps. Optical mal population of the lower energy level of the laser
windows to seal off the tube can be realized by plane transition would reduce the optical gain. In fact, for op-
transparent plates at the Brewster angle with respect timized cooling the glass tube should be as small as
to the beam axis. One polarization state of the laser possible without introducing significant aperture losses
light can pass through the Brewster window without by truncating the free-space laser beam. Typical diam-
unwanted reflections. Thus, the Brewster window also eters are 5–10 mm, depending on the tube length and
acts as a polarization-selecting element inside the laser the optical resonator design [11.1354].
resonator.
The CO2 –N2 molecule mixture can be excited Vibration and Rotation of the CO2 Molecule
inside the gas discharge by collisions with free elec- The emission wavelengths of the CO2 laser are deter-
trons [11.1351]. The excited roto-vibrational states mined by the vibrational and rotational energy levels of
provide optical gain at certain wavelengths in the in- the CO2 molecule, which are discussed in more detail in
frared. A simple plano-concave stable optical resonator [11.1355, 1356] or [11.1357]. All data in the following
with two mirrors located at each ends of the discharge sections are given for the naturally most abundant iso-
tube can be used to provide continuous laser oscillation. topologue 16 O12 C16 O. Figure 11.118 shows the three
The totally reflecting mirror is often made of copper, fundamental vibrational modes: the symmetric stretch
optionally with additional gold or protective dielectric mode v1 along the molecule axis, the bending mode v2
layers to enhance lifetime and reflectivity. The output with motion of the C atom in a plane perpendicular to the
coupler can be made of zinc selenide (ZnSe), germanium molecule axis, and the asymmetric stretch mode v3 . The
or silicon, as these materials have good transparency in bending mode is twofold degenerate because of the pos-
the mid-infrared, in contrast to common silica-based
glasses. The required reflectivity is provided by dielec-
tric coatings on the mirror substrate. As the optical
small-signal gain of the active CO2 gas medium is quite O C O
high compared to a helium–neon (HeNe) gas laser and
Symmetric stretch mode õ1
is in the range of 1 m−1 , reflectivities of output cou-
plers may range from 20% to 90%. Optimum output
coupler reflectivities for a maximum laser power are of-
O O
ten determined experimentally. Alternatively, they can C
be calculated by a so-called Rigrod analysis if param-
eters such as the small-signal gain and the saturation Bending mode õ2
intensity of the medium are known [11.1352, 1353].
Typical efficiencies ηE , defined as the ratio of the ex-
tracted optical laser power PL to the applied electrical O C O
Fig. 11.118 Vi-
power PE into the discharge, are in the range of 10%. brational modes
The largest part of the electrical excitation power is dissi- Asymmetric stretch mode õ3 of the CO2 mol-
pated as thermal energy inside the gas volume. To avoid ecule
728 Part C Coherent and Incoherent Light Sources

Even if there is no vibrational excitation present (all


Energy W
2 n i = 0) and the molecule is in its ground state there is
0
(20 0) 4
(04 0) 2 0 (12 0)
(12 0) energy stored inside the molecule that cannot be ex-
0 (04 0)
(04 0) 0
(00 1)
3
1
(11 0)
changed. Thus, this zero-point energy is neglected in all
1 (03 0)
(03 0) further energy formulas and diagrams.
0
(10 0) 0
2
(02 0) To characterize the vibrational state completely
(02 0)
another quantum number l is required to define the distri-
Part C 11.4

1 bution and the phase of the bending vibration quanta in


(01 0)
0 v2 into the two orthogonal coordinates. For each number
(00 0)
0
õ1 õ2 õ3 Combinations
n 2 there are n 2 + 1 values for the angular momentum l:

⎨n , n − 2, n − 4, . . . , 0 ; n even
Fig. 11.119 Some of the lowest vibrational energy levels of the CO2 2 2 2 2
|l| =
molecule. The Fermi resonance couples energy levels as indicated ⎩n , n − 2, n − 4, . . . , 1 ; n odd .
2 2 2 2
by the dashed lines
(11.123)

sible bending motions in the two orthogonal coordinates For example for n 2 = 2 the value l = 0 describes a linear
of the plane. bending motion, and l = −2 or l = 2 describes circular
In the classical model of the unperturbed harmonic motions of the C atom in opposite directions in the plane
oscillator each mode has an associated vibrational fre- perpendicular to the molecule axis. A vibrational state of
quency: the CO2 molecule is labeled with the common Herzberg
notation (n 1 nl2 n 3 ), for example (000 0) for the ground
f 1 = 40.51 THz, f 2 = 20.15 THz,
state or (122 0) for a state with simultaneous excitation
f 3 = 71.84 THz . (11.121) of several vibrational modes [11.1355].
In the quantum-mechanical model the energy of any Figure 11.119 shows the energies of some of the
vibrational state of the molecule can only have dis- lowest vibrational states. The energy levels observed by
crete values called the vibrational energy levels. Using emission and absorption of radiation, as shown in Ta-
the integer vibrational quantum numbers n 1 , n 2 and n 3 ble 11.38, are slightly different than those calculated
that describe the degree of excitation of the vibrational using the simple-harmonic-oscillator theory (11.122).
modes, the total vibrational energy Wv of the molecule More-precise calculations using anharmonic corrections
can be written as a sum over the single vibrations: and considering the mutual coupling of the three vibra-
tional modes are therefore required.
  The so-called Fermi resonance is of particular impor-
1
Wv = h f 1 n 1 + + h f 2 (n 2 + 1) tance for the laser process in the CO2 laser. Vibrational
2
  states with equal values of the term 2n 1 + n 2 and l = 0
1
+ h f3 n3 + . (11.122) have almost the same energy and are strongly coupled.
2 Due to this Fermi resonance the (100 0) state is shifted up

Table 11.38 Labeling, symmetry/parity classification and energies of some low-lying vibrational states of the CO2
molecule [11.1358]
State Frequency and energy
Herzberg AFGL Type ν̄ (cm−1 ) f (THz) W (meV)
(000 0) 00001 Σ+
g 0 0 0
(011 0) 01101 Πu 667.380 20.008 82.745
(020 0) 10002 Σ+
g 1285.408 38.536 159.370
(022 0) 02201 ∆g 1335.132 40.026 165.535
(100 0) 10001 Σ+
g 1388.184 41.617 172.113
(031 0) 11102 Πu 1932.470 57.934 239.596
(033 0) 03301 Φu 2003.246 60.056 248.371
(111 0) 11101 Πu 2076.856 62.263 257.497
(000 1) 00011 Σ+
u 2349.143 70.426 291.257
Lasers and Coherent Light Sources 11.4 The CO2 Laser 729

Fig. 11.120 Rota- equals the energy difference ∆W = W2 − W1 between


tion of the CO2 two given energy levels of the respective atom or
molecule O C O molecule. Additionally, selection rules based on the con-
servation of the spin or angular momentum and due
to symmetry properties of the wave functions have
to be considered. Based on the formalism of vibra-
and the (020 0) state is shifted down in energy. The popu- tional matrix dipole elements only certain transitions

Part C 11.4
lation densities of these states are quickly exchanged by are allowed [11.1357]. The strongest allowed CO2
collisions with each other. Also the quantum-mechanical laser emission lines result from the vibrational transi-
wave functions and the vibrational motion of the two re- tions (000 1) → (100 0) centered at wavelengths around
sulting levels are a strong mixture of the unperturbed 10.4 µm (10 µm band) and (000 1) → (020 0) around
vibrational states. In the CO2 laser literature the re- 9.4 µm (9 µm band). For these regular transitions the
sulting levels are sometimes labeled (I) for the more following selection rule for the rotational quantum num-
(100 0)-like state and (II) for the more (020 0)-like state. bers of upper and lower energy levels apply:
Spectroscopic databases, which are an excellent refer-
∆J = J2 − J1 = ±1 . (11.126)
ence for accurate absorption and emission wavelengths
of the CO2 molecule, often use a different labeling For a given lower rotational state J1 there are two
scheme than the simple Herzberg scheme, for example different possibilities for the emission of photons, as
the so-called AFGL (Air Force Geophysics Lab, USA) shown in Fig. 11.121. Transitions are named after the
notation, which gives a better treatment of the Fermi rotational quantum number of the lower state. Addi-
resonance [11.1359, 1360]. tionally, the transitions are labeled P (the P branch)
Superimposed onto the vibration is the rotational for ∆J = −1 and R (the R branch) for ∆J = +1. For
motion of the CO2 molecule, as shown in Fig. 11.120.
Only the rotation around an axis perpendicular to the
molecule axis has a significant moment of inertia and J2
is considered further. The discrete energy levels in the
rigid-rotator model are given by
Wr = B · J(J + 1) , (11.124)

where B is the rotational constant and J is the quantum


number for the rotational state. The higher the value of 25
23
J the faster would be the rotation of the molecule in the 21
19
classical mechanical model. For the (000 1) vibrational
state, for example, B has a value of 9
(0001)
B = 48.0 meV = h f r = h 11.6 GHz . (11.125) J1 NJ

More precise calculations show that the rotational con- J1


10P20
stant B is slightly dependent on the vibrational state
10R20
because of the anharmonicity and also dependent on the
rotational quantum number J itself because of centrifu- 9P20
gal forces. 9R18
The total internal energy W = Wv + Wr of the CO2
22
molecule is the sum of the vibrational and the rotational 20
18 22
energies. The energy stored in the rotational motion 20
is usually much smaller than in the vibration motion. 18
(1000)
Thus, the rotational energy levels can be thought of as NJ
superimposed on each vibrational level. (0200)
NJ

Emission Lines of the CO2 Laser Fig. 11.121 Examples of names for allowed roto-vibrational
Absorption, spontaneous and stimulated emission of transitions of the regular bands. The rotational distribution
light can occur when the energy of a photon Wp = h f p is calculated for T = 400 K
730 Part C Coherent and Incoherent Light Sources

Fig. 11.122 Calculated relative small-


Frequency f (THz)
signal gain for the regular bands of
33 32 31 30 29 28 27
Relative small the CO2 laser at T = 500 K
signal gain g0 10R 20 10P
9R 9P 20
20 20

10
10 40
Part C 11.4

10
10 40
40 40

9 9.5 10 10.5 11 11.5


Wavelength ë0 (µm)

example one of the strongest emission lines of the Besides of the regular bands, there are other vibra-
CO2 laser is labeled 10P(20), indicating a transition tional transitions with slightly shifted wavelengths that
from the 10 µm band with the lower rotational state can be operated as lasers: the so-called hot band and
J = 20 and ∆J = −1. Different transitions have differ- sequence band. Table 11.39 shows a summary of vi-
ent energy differences ∆W and thus different emission brational transitions. For laser emission in the sequence
frequencies f or wavelengths λ because of the non- or hot bands, lasing in the regular bands must be sup-
equidistant rotational energies in (11.124). This is the pressed, for example by passive absorption cells filled
origin of the multitude of possible emission lines of the with hot CO2 gas inside the resonator [11.1347]. Almost
CO2 laser. all technical lasers operate in the regular bands.
Figure 11.122 shows the calculated relative gain of The optical small-signal intensity gain per unit
the regular bands of a typical CO2 laser. Both vibrational length g0 of a given transition is proportional to the
transitions have characteristic R and P branches due to population density difference of the upper and the lower
the superimposed rotational energy levels and the selec- states, weighted with the respective degeneracy factors:
tion rules. Exact line positions are listed in [11.1347] 2J2 − 1
based on [11.1361], or in spectral databases such g0 ∼ (Nn 2 J2 − Nn J ) . (11.127)
as [11.1359], which also lists transition dipole moments 2J1 − 1 1 1
that are useful for the calculation of the absorption and The population densities Nn J are the numbers of
gain of a transition [11.1362]. Note that in Fig. 11.121 molecules per unit volume in the roto-vibrational energy
only rotational states of even order J are present for level n and J. Within each vibrational state n with a total
the lower states (100 0) and (020 0). The odd states are population of Nn the distribution of the molecules in the
missing because of the symmetry properties and parity different rotational states Nn J is described by a thermal
rules (Σ+g ) of these states in the
16 O12 C16 O isotopo- Boltzmann distribution, weighted by the total rotational
logue [11.1356]. Similar considerations are valid for the partition sum and the degeneracy factor for each J:
upper state of the regular band (000 1) (Σ+    
u state), which 2B Wr
only has odd rotational quantum numbers J. Nn J = Nn (2J + 1) exp − , (11.128)
kT kT
Table 11.39 Possible vibrational lasing transitions with the translational gas temperature T and the Boltz-
mann constant k. The rotational level at the maximum of
Vibrational band Comment
this distribution at a given temperature can be approxi-
(000 1) → (100 0) Regular band, 10 µm
mately calculated as
(000 1) → (020 0) Regular band, 9 µm 
(011 1) → (111 0) Hot band kT 1
Jmax ≈ − . (11.129)
(011 1) → (031 0) Hot band 2B 2
(000 2) → (100 1) Sequence band For typical gas temperatures of T = 400 K the levels
(000 2) → (020 1) Sequence band around J = 19 have the strongest population. In CO2
Lasers and Coherent Light Sources 11.4 The CO2 Laser 731

lasers without any further wavelength-selective elements citation the population of the upper laser state (000 1)
normally only one transition around the 10P(20) line is always smaller than the lower laser levels (100 0)
at a wavelength of 10.59 µm will lase, as this one has or (020 0). This is the normal case for passive media,
the strongest gain (Fig. 11.122). Typical values for the which show absorption lines on the respective transition
small signal gain g0 are in the range from 0.5 m−1 wavelengths.
to 1.5 m−1 . To achieve an inversion, and thus optical gain, in
Even under lasing conditions the rotational distribu- an active medium an electrical gas discharge is usu-

Part C 11.4
tion will maintain its thermal Boltzmann shape because ally used to excite the CO2 laser. Accelerated electrons
of fast population exchange between the rotational lev- inside the discharge collide with the molecules and
els by molecule collisions. Thus, almost all rotational lose part of their kinetic energy. This energy can be
states within the upper vibrational level can contribute transformed into vibrational excitation energy of the
to a single lasing transition rather than just the popula- molecules or into kinetic energy by a pure transla-
tion of the particular upper level, for example the J = 19 tory motion. How effective a certain vibrational state
state of the (000 1) vibrational level. This affects mainly of the molecule is excited is described by the excita-
the saturation intensity Is of the optical gain, which is tion cross section, which is dependent on the energy of
much larger than expected form the population Nn J of the electrons. For inversion of the regular CO2 laser
a single rotational level J itself. The saturation inten- lines, a selective population of the upper laser state
sity Is is in the range from 100 W cm−2 for sealed-off (000 1) is required. This is barely possible in a pure
large-bore DC-excited lasers to over 1000 W cm−2 for CO2 gas discharge as the cross sections for excitation of
fast-flow systems. the different vibrational states are of the same order of
magnitude.
Electrical Excitation and Gas Composition Therefore, nitrogen (N2 ) is added to the laser
Without any excitation and in thermal equilibrium gas [11.1351]. As a molecule with two atoms it only
the population of the vibrational states is given by has one vibrational mode. As a homonuclear molecule
a Boltzmann distribution. As the energies of the lower it has no electric dipole moment and hence, no radiative
vibrational levels are almost of the same order as the decay of excited vibrational states. Thus, nitrogen can
thermal energy kT = 25.5 meV at 296 K, the thermal efficiently store energy in its vibrational excited states.
population of levels above the ground state cannot be ne- More than 50% of all N2 molecules can be excited to
glected. The population Nn of a given vibrational level higher vibrational levels inside a gas discharge. The first
n is given by: excited vibrational state, n = 1, has nearly the same en-

ergy (289 meV) as the upper laser level (000 1). Due to
exp − dnkTWn resonant collisions between excited nitrogen atoms vi-
Nn = N0 , (11.130) brational energy is readily transferred to the desired CO2
Q vib
state
where N0 is the total density of CO2 molecules, dn is
the degeneracy factor and Wn the energy of level n, and N2 (n) + CO2 (000 0)
Q vib is the vibrational total partition sum. Without ex-  N2 (n − 1) + CO2 (000 1) + ∆W . (11.131)

õ 1, T 1 õ 2, T 2 õ 3, T 3 õ, TN õCO, TCO
O O
O C O C O C O C N C O
V–V

(0001) (1)
V–T Laser (1)

10 µm
Collision 9 µm
(1000) (0200)
e– e– e–
1
(01 0)
Emission
(0000) (0) (0) Fig. 11.123 Energy-level diagram of
CO2 N2 CO the CO2 laser process with excitation
and decay paths
732 Part C Coherent and Incoherent Light Sources

The energy difference ∆W = −2.2 meV  kT is eas- temperature T they form the so-called five-temperature
ily available from the thermal kinetic energy of the model of the CO2 laser. This model can be used to
molecules. quantify the degree of vibrational excitation in a given
Figure 11.123 shows the energy-level diagram of the laser system and to calculate the optical gain of different
CO2 laser process. Accelerated electrons from the gas transitions [11.1347, 1363, 1364].
discharge excite nitrogen molecules to higher vibrational Note that the vibrational temperatures inside a gas
levels by collisions. These excited nitrogen molecules discharge can be significantly higher than the usual phys-
Part C 11.4

transfer their energy to the upper laser level (000 1) of ical gas temperature T which describes the translatory
the CO2 molecule and provide a significant population kinetic energy. For typical laser conditions the temper-
inversion compared to the lower laser levels. From there, atures T3 and TN can be in excess of 1000 K, even if
two strong lasing transitions by stimulated emission of the physical gas temperature T is only 450 K, for exam-
photons are possible, the 9 µm band with (020 0) as the ple. This describes the desired high level of excitation
lower laser level and the 10 µm band with (100 0). of these modes for a strong inversion, especially if there
To maintain a large inversion thermal population of is no laser action to reduce the population in (000 1)
the lower laser levels must be avoided by efficient cool- by stimulated emission. The vibrational temperatures
ing of the laser gas. Therefore, helium (He) is added to T1 and T2 are almost equal because of their coupling
the laser gas. Helium is the gas with the largest ther- and are slightly larger than the physical temperature, be-
mal conductivity. It also plays an important role for the cause their population decay to the ground state takes
population decay of the (020 0) and (011 0) levels by place with a finite rate. Here, as low as possible vibra-
vibrational–translational (V–T) relaxation. Thereby, vi- tional temperatures are desired for a low population of
brational energy of the CO2 molecule is transferred to the lower laser levels. Of course, no vibrational temper-
kinetic energy, the translatory motion of the molecules. ature can be lower than the physical gas temperature T .
Radiative decay by spontaneous emission is also pos- It is also the temperature T that is valid for the rotational
sible for the (020 0) and (011 0) levels, but not for the population distribution.
(100 0) level, which shows no change in the dipole mo- Thus, a gas mixture for a CO2 laser could be
ment during vibration. It can reduce its population by He : N2 : CO2 = 8 : 2 : 1, with large individual variations
V–T relaxation directly to the (011 0) level, but also by between specific laser designs, which are often exper-
the Fermi resonance via collisions and energy exchange imentally defined for maximum laser output. The gas
with the (020 0) state. In fact, the degree of vibrational pressure p is typically a few tens of hPa for longitudi-
excitation of these two vibrational modes is almost the nally DC-excited lasers, in the range of 100 hPa for lasers
same due to this Fermi coupling. After relaxation to the with a transversal RF discharge or can equal the atmo-
ground state (000 0) the CO2 molecule is available for spheric pressure in so-called TEA (transversaly excited
excitation and the laser process again. atmospheric pressure) lasers with a pulsed transversal
Within one vibrational mode, for example v1 of the discharge. The gas pressure influences the stability of
CO2 molecule, there is a strong interaction of the vibra- the gas discharge and the electric field strengths required
tional levels by vibrational–vibrational (V–V) relaxation to start and maintain a stable discharge at the dif-
and excitation processes during collisions: ferent excitation frequencies and geometries. Together
with the applied electric field E inside the discharge
CO2 (n 1 ) + CO2 (n 1 ) the gas pressure p affects the electron energy distri-
 CO2 (n 1 + 1) + CO2 (n 1 − 1) + ∆W , (11.132) bution function (EEDF). For efficient excitation of the
desired vibrational nitrogen states electrons with ener-
where the small energy difference ∆W coming from gies of 2–3 eV are required, where the effective cross
the anharmonic forces can almost be neglected. By this section for vibrational excitation of N2 has a maxi-
fast thermalization the population distribution of the vi- mum [11.1347].
brational levels within one mode vi can be described
by a Boltzmann distribution similar to (11.130) with Dissociation and Gas Additives
a specific vibrational temperature Ti for this particu- The complex-shaped electron energy distribution func-
lar mode. Three vibrational temperatures T1 , T2 , and tion (EEDF) in such a laser gas discharge always has
T3 are required to describe the three vibrational modes a tail extending to quite high electron energies. These
of the CO2 molecule. Together with the vibrational electrons can start unwanted chemical dissociation pro-
temperature of the nitrogen TN and the physical gas cesses of the CO2 molecule inside the gas discharge, for
Lasers and Coherent Light Sources 11.4 The CO2 Laser 733

example gases react inside the gas discharge, for example with
CO2 + e − −
 CO + O , ∆W = − 3.85 eV ,
oxygen radicals to form hydroxyl radicals OH. This
(11.133)
hydroxyl radical is an efficient catalyst for oxidizing
− −
CO back to CO2 . On the other hand, water vapor with
CO2 + e  CO + O + e , ∆W = − 5.5 eV . its multitude of vibrational states rapidly deexcites the
(11.134) upper laser state (000 1) and quenches the desired pop-
This is the origin of the complex gas chemistry that ulation densities of this level. The reported water vapor

Part C 11.4
leads to a reduced CO2 concentration and the forma- concentrations for optimum catalysis and yet low vi-
tion of a significant CO concentration inside the laser brational quenching are quite low [11.1347] and were
gas tube [11.1367]. By the law of mass action a typical found to be hard to control in real laser systems. In
equilibrium ratio of 1 : 1 between CO2 and CO is estab- other laser systems no clear proof of an optimum wa-
lished if no means to reduce the dissociation are present. ter vapor content was found at all [11.1372, 1373]. As
Clearly this reduces the overall laser output power and a rule of thump the dew point of the laser gas should
efficiency. be below −40 ◦ C, equivalent to a water vapor partial
In lasers with a steady gas exchange by a gas flow pressure of 0.13 hPa. Creeping of water from the cool-
the laser gas can be replaced by fresh gas from a premix ing system has to be avoided. However, some laser gas
bottle or can be partially regenerated by forced circu- premixes may contain small amounts of hydrogen, as
lation through catalysts to prevent too high a degree deemed appropriate by the manufacturer of the laser
of dissociation. Naturally, the gas dissociation is more system.
crucial for sealed-off lasers without any gas exchange. Other gas premixes include carbon monoxide (CO)
To decrease dissociation processes and maintain a high or oxygen (O2 ). By the law of mass action both additives
output power, many different gas additives to the basic can shift the equilibrium of the dissociation reactions
mixture have been studied [11.1347]. Table 11.40 shows (11.133) and (11.134) towards the left. Too high an
the composition of some commercial laser gas premixes O2 concentration has a detrimental influence on the
for high-power CO2 lasers. discharge stability and the EEDF, as it is a strongly
Xenon (Xe) is without doubt the most effi- electronegative gas. CO as a diatomic molecule has sim-
cient and most widely used additive for sealed CO2 ilar vibrational energy levels to nitrogen and can also
lasers [11.1368–1370]. Xe has a first ionizing poten- transfer vibrational energy by resonant collisions to the
tial of 12.1 eV, which is some eV less than the other upper laser state of the CO2 molecule (Fig. 11.123). An-
gases. Hence, the same current density in the discharge other benefit of adding CO and O2 initially to the gas
can be maintained at a lower applied electric field. This premix for filling the laser is that the gas is already
in turn shifts the EEDF towards lower energies, which near its equilibrium composition for the dissociation
are more efficient for vibrational excitation, and there process, so no overshoot or undershoot of the laser
are fewer fast electrons to cause dissociation processes. power occurs when the laser is operated for the first
On the other hand, Xe with its heavy atomic weight has time after filling. However, CO is not as effective as ni-
a very low thermal conductivity. Also it is a very rare trogen for vibrational excitation. The energy difference
and expensive noble gas. Sealed laser mixtures typically from the CO:(n = 1) vibrational level to the CO2 :(000 1)
contain a few percent of Xe. level is 25.5 meV and is thus larger than with nitro-
Water vapor (H2 O) and molecular hydrogen (H2 ) gen. Additionally, CO has allowed dipole transitions
have also been extensively studied [11.1347,1371]. Both to the ground state by spontaneous emission, which

Table 11.40 Some commercial gas premixes for different industrial CO2 laser types [11.1365, 1366]
Premix name / Composition Laser type,
(Maker) He N2 CO2 CO O2 Xe H2 model series
Lasermix  322 65.5 29 5.5 Fast axial-flow,
(Linde AG) Trumpf TLF Series
Lasermix 690 65 19 4 6 3 3 Diffusion-cooled sealed-off,
(Linde AG) Rofin Slab DC 0XX
LasalTM 81 80.8 15 4 0.2 DC excited slow-flow,
(Air Liquide) FEHA SM Series
734 Part C Coherent and Incoherent Light Sources

decreases vibrational excitation compared to nitrogen. the oxygen in the volume. This shifts the equilibrium
Also CO is the only toxic gas of the species discussed of the dissociation towards lower CO2 content in the
here. Care has to be taken when handling such gas tube. Therefore, uncoated copper is not well suited
mixtures. as a material in direct contact with the gas discharge.
Away from the discharge, however, copper is an excel-
Materials for CO2 Lasers lent material for mirrors. Copper mirrors can be cooled
Materials for the laser tube have to be chosen properly. effectively by water channels from the rear side. This
Part C 11.4

All common rules for building and preparing vacuum is important for resonator and deflecting mirrors in-
systems apply. Materials with low out-gasing and low side high-power lasers. For example, with an output
vapor pressure must be used. This normally inhibits the coupler reflectivity of 50% the circulating light power
application of plastics and polymer-based glues in CO2 inside the resonator is twice the rated laser power of
laser tubes. Additionally, the UV radiation of the gas the system. Even if the infrared reflectivity is very high,
discharge will degrade most organic compounds rapidly. this can lead to considerable warming and mechanical
There are only a few epoxy-based adhesives that may be stress if the mirrors are not cooled. Copper can be elec-
used. troplated with nickel (Ni) and then coated with gold
Many low-power sealed-off lasers and even high- (Au). This makes the copper surface more stable against
power lasers with slow or fast gas circulation use quartz oxidation.
glass tubes to confine the laser gas. Quartz (SiO2 ) glass
is thermally stable, chemically inert, robust against UV Catalysts and Gas Analysis
radiation and has low dielectric losses. However, silica- Much research was carried out to find proper cata-
based glasses have high infrared absorption, even for lysts to reduce the dissociation of CO2 and to maintain
grazing incidence of light to the surface. Thus, the diam- a high output power. In lasers with a gas flow, the
eter of the quartz glass tube needs to be considerably laser gas can be circulated through external catalysts.
larger than the laser beam formed by the resonator mir- Common catalysts such as hot platinum [11.1376] or
rors. For waveguide lasers (see Sect. 11.4.2) tubes made platinum on metallic oxides such as tin oxide with a large
from other materials must be used. Alumina (polycrys- surface area [11.1377,1378] can be used. However, fast-
talline Al2 O3 ceramics) is often used. It is a dense and flow systems require gas replenishment of a few liters
vacuum-tight ceramic material, which is also dimen- per hour to compensate for residual vacuum leaks or
sionally and thermally stable. Its infrared absorption is material contamination. As the price of the laser gas
lower than quartz glass, making it suitable for hollow mixture is rather low compared to the costs of installing
dielectric waveguides. Also it has very low dielectric a catalyst, they are usually not applied in fast-flow
losses at radio frequencies, making it an ideal mater- systems.
ial for transversal capacitively coupled RF discharge For sealed lasers without any gas flow the sit-
excitation. uation is quite different. The dissociation reactions
Good material choices to confine the gas vol- inside the gas discharge are fast and equilibrium
ume are also inert passivated metals such as stainless is reached in a tenth of a second within the dis-
steel [11.1374] and passivated aluminium. Steel can charge. On the other hand, diffusion time constants
easily be welded, both with conventional techniques or to a nearby gas reservoir are in the range of min-
with lasers, to built a vacuum-tight laser tube. Weld- utes. Thus, any catalytic surfaces need to be in close
ing of aluminum is more difficult. On the other hand, contact with the discharge itself. For example, cat-
aluminum has a far better thermal and electrical con- alytic active platinum cathodes [11.1371] and distributed
ductivity and a higher infrared reflectivity. This makes platinum [11.1379] or sputtered gold coatings on
aluminum a very good material for waveguide plates and the inside of a longitudinal discharge tube [11.1380]
electrodes for transversal RF discharges [11.1375]. have been reported. For waveguide lasers, gold-coated
Electrolytic copper or oxygen-free high-conductivity electrodes were found to be effective in some re-
(OFHC) copper can also be used because of their ex- ports [11.1381, 1382]. The catalytic activity and the
cellent thermal and electrical conductivity and infrared advantages for laser output power of these approaches
reflectivity. On the other hand, copper can be oxidized depend on the preparation of the catalytic surfaces, the
by oxygen radicals from the dissociation process in- gas composition and the laser geometry itself, leaving
side the gas discharge. Copper does not form stable, open many questions and an impression of alchemy.
inert oxides on its surface but rather absorbs and binds Some commercial laser designs embody some sort of
Lasers and Coherent Light Sources 11.4 The CO2 Laser 735

these techniques, as deemed best for the given laser


Emission counts (arb. units)
design.
1 + 1
To study the effects of catalysts on the gas com- 3 + 3
CO: B Ó ® A Ð
CO: b Ó ® a Ð 1–0 0–0 0–1 0–2 0–3 0–4
position or, more generally, to have more data about 0–0 0–2 0–4
1–1
the active medium such as rotational and vibrational 0–1 0–3 0–5
temperatures various methods can be applied. Mass 3
N 2: C Ð u ® B Ð g
3 N2 N2 N2
spectrometers are commonly used for gas analysis.

Part C 11.4
He
However, short-lived species from the discharge can- He He He+ He He He+ He He He
not be easily measured. The required pressure reduction Xe Xe Xe
from some tens of hPa down to 10 × 10−7 hPa tends
to change the original gas compositions. Special tech-
niques in experimental laser systems have been used
to measure gas compositions directly from the gas dis-
charge, and have given insight into the complex gas
chemistry [11.1367, 1384].
Another method is to study the visible and UV 200 300 400 500 600 700 800
Intensity Wavelength (nm)
spontaneous emission from electronically excited states
1/10 scaled
inside the gas discharge [11.1385]. This can even be
done with the naked eye. Figure 11.124 shows an ex- Fig. 11.124 Visible spectrum the sidewards spontaneous emission of
ample spectrum. A gas discharge without much CO a CO2 laser gas discharge (after [11.1373, 1383])
appears pink or redish-purple because of vibronic nitro-
gen emission lines in the red and blue visible spectrum. Output Spectra and Line Broadening
With a significant carbon monoxide content there are Due to the fast population relaxation between the rota-
additionally some CO emission lines spread over the tional levels only the rotational transition with the largest
visible and a strong emission band in the blue–UV gain is usually observed. A similar competition as for
spectral region. Thus, a gas discharge with a higher the rotational lines is also given for the two regular vi-
degree of dissociation looks more blueish-white. The brational transitions. As both have the same upper laser
color change can be observed in slow-flow DC-excited level (000 1), and the population levels of the lower states
gas lasers with glass tubes from the gas inlet to the (100 0) and (020 0) are coupled by the Fermi resonance
gas outlet, for example. For quantitative studies fiber- and have similar decay rates, only the vibrational tran-
coupled spectrometers with fast readout can be used to sition with the largest gain will survive. Typically this is
gain time-resolved concentration data [11.1383]. With the 10P(20) transition or one of its neighbors for many
high-resolution spectroscopy, for example of the UV ni- lasers.
trogen emission band, the rotational temperatures of the Every roto-vibrational transmission line is broad-
gas can be measured. Using an imaging system, spatially ened by several broadening mechanisms. At gas pres-
resolved data for these parameters have even been meas- sures above 10 hPa collisional or pressure broadening
ured in the discharge gap of an RF-excited high-power dominates over Doppler broadening. The collision-
slab laser [11.1386]. broadened line shape is described by a Lorentzian
Absorption spectroscopy with tunable diode lasers function having a line width (FWHM) ∆ f L proportional
is also very effective for measuring species concentra- to the total gas pressure p:
tions and roto-vibrational temperatures directly inside  
the laser tube or gas discharge. To do this, a wavelength- ∆ f L = 2 p ψCO bCO + ψN bN + ψHe bHe
2 2 2 2
tunable diode laser is adjusted to the various absorption  
transitions of the relevant molecules (i. e., CO2 , CO, 300 n
× (11.135)
N2 O, NO). By aiming the diode-laser beam through T
the gas volume and measuring the relative intensi- where the ψi are the fractions of the respective gases
ties of several rotational and vibrational transitions and T is the gas temperature. The temperature exponent
an accurate diagnostic of the active medium is possi- n is 0.58 for constant pressure [11.1393], with values
ble [11.1387–1391]. Recently, the catalytic activity of ranging from 0.5 to 0.7 also found in the literature. The bi
special gold coatings on electrodes for RF-excited slab are the pressure-broadening coefficients resulting from
lasers was verified using this technique [11.1392]. collisions with species i and are given in [11.1393] to
736 Part C Coherent and Incoherent Light Sources

Normalized gain and loss


have significantly lower efficiencies for several reasons.
Line center f0 The electrons inside the gas discharge do not only excite
the required vibrational states of the molecules but also
Small-signal gain other states. Also a significant part of the kinetic elec-
tron energy is transferred into pure translatory motion
Saturated gain of the molecules and thus transferred into heat. Addi-
tional energy is lost in the ionizing processes required
Part C 11.4

Resonator losses to maintain the gas discharge and in chemical disso-


ciation processes. Also not every vibrationally excited
molecule contributes to the laser process. Vibrational
Normalized frequency (f- f0)/ÄfL energy decays by vibrational–translational relaxation,
Lasing frequency which produces heat again and by radiative decay by
Äfq spontaneous emission of excited states. Finally, optical
Longitudinal resonator eigenfrequencies fq energy is dissipated in absorption losses of the mirrors
and waveguides or by limited aperture diameters.
Fig. 11.125 Homogeneous saturation of a Lorentzian gain Typical electrical efficiencies ηE , defined as the ratio
profile leads to lasing of a single longitudinal resonator of the extracted laser power PL to the electrical power PE
eigenfrequency applied directly to the discharge tube, are in the range of
10% for slow-flow DC-excited laser, up to 15% for RF-
be: excited waveguide lasers and up to 20% for fast-flowing
systems. The overall wall-plug efficiencies ηtot as a ratio
bCO = (3.40 − |m| · 0.0272) MHz hPa−1 (11.136)
of laser power PL to mains supply power Pmains are
2

bN = (2.35 − |m| · 0.0127) MHz hPa−1 (11.137) always lower than ηE . This is due to conversion losses
2 in the electronic power supplies to provide the required
bHe = (1.77 − |m| · 0.00083) MHz hPa−1 , DC high-voltage or RF power. A considerable amount
of energy is also dissipated in the gas circulating system
(11.138)
of fast-flow lasers.
where m = −J for the P branch and m = J + 1 for the The output power of a given CO2 laser can be
R branch. For example, the most common 10P(20) line roughly estimated by simple thermodynamics. If all
at 100 hPa and 500 K in Lasermix 322 from Table 11.40 aspects of optical design, electrical excitation and gas
has a Lorentzian line width (FWHM) of 284 MHz. The composition are optimized, electrical efficiencies ηE as
Doppler line width at this temperature would be ∆ f D = discussed above can be assumed. From this point, the
36.2 MHz and can be considered if a Voigt line shape laser power is finally limited by the cooling and heat re-
instead of a pure Lorentzian is used [11.1394]. moval capacity of the laser system. The power dissipated
Within this line width one or more longitudi- by the electric excitation Pdiss should not heat the laser
nal resonator eigenfrequencies f q may be located. gas above a certain temperature, for example 450 K.
For an example length for a CO2 laser resonator In diffusion-cooled lasers no forced gas flow con-
of L res = 2 m a spacing of the eigenfrequencies tributes to the heat removal. The thermal conductivity
∆ f q = c/2L = 75 MHz results. As the collision- of the gas mixture and the diffusion of excited vibra-
broadened line saturates homogeneously, only the tional states to the housing walls determine the thermal
eigenfrequency closest to the center frequency of the transport processes. For a given tolerable temperature
transition can lase in the steady state after saturation, rise ∆T of the laser gas in the discharge area, the max-
as shown in Fig. 11.125. Thus, CO2 lasers are typically imum applicable dissipated thermal power Pdiss can be
longitudinally single-mode lasers. calculated by solving the differential heat-transfer equa-
tion for the given geometry. For fast-flowing systems
Efficiency, Output Power and Cooling the amount of heat removal is given by the specific heat
The theoretical limit for the efficiency of a laser is the capacity c P of the gas and the mass flow ṁ.
internal quantum efficiency ηq . For the CO2 laser this With the assumption that almost all electrical exci-
is the ratio of the energy of the laser photons to the en- tation power PE is finally dissipated into heat Pdiss , the
ergy of the upper laser level (000 1) and is roughly 40%. maximum permissable excitation power PE,max for the
This is quite high for a gas laser. Real technical lasers given temperature rise ∆T is thus known. The maximum
Lasers and Coherent Light Sources 11.4 The CO2 Laser 737

possible output power PL,max of this laser system can General design aspects are: as efficient a heat removal
then be calculated with the assumed electrical efficiency as possible, a compact optical resonator for a small foot-
ηE . This exaggerates the importance of the cooling meth- print even at very high power levels and a rugged and
ods for high-power lasers. Different approaches will be robust design for maintenance-free long-term industrial
discussed in the next section on technical lasers. operation.
More-exotic laser types such as optically pumped
11.4.2 Typical Technical Designs CO2 lasers, black-body radiation-pumped lasers, lasers

Part C 11.4
with electron-beam sustained gas discharges and gas-
Although CO2 lasers with a longitudinal DC discharge dynamic CO2 lasers are not further considered in detail
inside a glass tube as described in Sect. 11.4.1 are still here.
being used and sold because of their simplicity, many
other types and realizations of the CO2 laser have been DC-Excited Fast-Axial-Gas-Flow Lasers
developed over the last decades. They can by systemat- Longitudinally DC-excited lasers have the advantage of
ically categorized according to various characteristics, a rather simple and cost-effective design. Modern DC-
as below. excited lasers use sophisticated electronically regulated
high-voltage (HV) supply circuits with both voltage and
Gas flow inside the laser. current control to omit the ballast resistor shown in
• No gas flow, sealed-off Fig. 11.117. This reduces ohmic losses in the HV circuit.
• Quasi-sealed-off, periodic gas exchange Vacuum-tube-based or more modern semiconductor-
• Slow gas flow axial to the laser beam based current regulators and switched-mode voltage
• Fast gas flow axial to the laser beam converters are applied.
• Fast gas flow transversal to the laser beam For high-power lasers a fast axial gas flow can be
used to cool the gas. Lasers with a power in the kW
Gas cooling. range [11.1396, 1397] were demonstrated in the late
• Diffusion-cooled, cooled walls of the gas discharge 1970s. Figure 11.126 shows an example of a modern
• Fast gas flow with external heat exchanger DC-excited fast-flow high-power laser. The gas dis-
charge in the gas tube is divided into four independent
Electrical excitation. sections to keep the required high-voltage levels mod-
• Longitudinal DC discharge, continuous erate. Two of the discharge and flow tubes shown can
• Transversal DC discharge at high gas pressure, be used in parallel, with a U-shaped folded light path
pulsed and resonator to double the length of the active medium.
• Capacitively coupled transversal RF discharge This is because the output power scales with the length
• Inductively coupled RF discharge of the gain medium.
• Microwave-excited gas discharge
Rear mirror Discharge Output coupler
Optical resonator. DC HV supply Glass tube
• Stable optical resonator Cathodes
• Unstable optical resonator
• Free-space propagation between the mirrors Anode Anode Anode
Gas flow
• Optical waveguide between the mirrors Gas distributor
• Combinations of these in different planes
Resonator mount
In principle, almost any of these characteristics could
Gas pre-cooler
be combined to give specific advantages. The three axes Gas pre-cooler
Heat exchanger
of the optical laser beam, the gas flow and the exciting
electrical field can be mutually parallel or orthogonal in
general. Some of the most important designs with their Cooling water
specific technical characteristics are discussed further Turbo blower

in the next sections. Commercial manufacturers of CO2


lasers often have quite different approaches, also de- Fig. 11.126 Longitudinally DC-excited high-power CO2 laser with
pending on their own intellectual property and patents. fast axial gas flow [11.1395]
738 Part C Coherent and Incoherent Light Sources

As discussed in Sect. 11.4.1, the maximum output sections. The additional heat resulting from the gas com-
power of a CO2 laser is also largely determined by pression by the turbo blower is removed by pre-coolers
its heat removal capacity. A fast gas circulation can be before the gas enters the discharge tube again.
driven by a turbo blower. From thermodynamic consid- Besides the fast gas flow there is also a permanent
erations, the maximum laser power PL,max of a fast-flow slow gas exchange with a fresh gas mixture, for example
laser can be calculated with a given electrical efficiency at a rate of 37 l (standard pressure and temperature) per
ηE : hour in a ratio He : N2 : CO2 = 25 : 12 : 2 for a particular
 
Part C 11.4

ηE commercial system. Longitudinally DC-excited lasers


PL,max = ηE PE,max = Pth up to several kW laser power are available. Depending on
1 − ηE
  the laser power and the application, such laser systems
ηE
= ṁ cp ∆T , (11.139) can emit a mixture of an ideal TEM00 mode and a hybrid
1 − ηE TEM∗10 donut-shaped mode.
where PE,max is the maximum applicable electrical
power, Pth is the thermal power dissipated in and RF-Excited Gas Discharges
removed from the discharge, ṁ is the mass flow, Radio-frequency (RF) excitation of the gas discharge
cp is the specific heat of the gas mixture, typically is widely used in CO2 lasers. In this context RF means
2500 J kg−1 m−3 , and ∆T is the maximum gas temper- a frequency range of roughly 1–500 MHz. Figure 11.127
ature rise that can be tolerated, typically 250 K. It can shows cross sections of typical geometries found in CO2
be seen clearly that the laser power scales with the mass lasers. In capacitively coupled RF (CCRF) discharges
throughput and thus with the flow velocity, which is lim- the electric field is applied by two metallic electrodes
ited by the onset of turbulence and the speed of sound. with the gas volume in between. The electric field E
For an assumed efficiency of PE = 15%, one yields an in the volume of the gas is sufficiently high to start
approximate required mass flow of 0.1 kg/s per kW of and maintain a self-sustained glow discharge [11.1350].
laser power. The heat dissipated in the gas is removed by The RF voltage URF and the RF electric field E are
a heat exchanger after the gas has passed the discharge typically applied transversally to the laser beam. Thus,
much lower voltages URF are required compared to
longitudinally excited discharges. URF is roughly 100 V
a) b) per mm discharge gap width d, depending largely on the
IRF Electrodes IRF
Electrodes gas pressure.
The electrodes can be electrically insulated from the
Discharge discharge by a dielectric material, for example a glass or
URF E Discharge E d
Insulator alumina tube as shown in Fig. 11.127a. No direct contact
Boundary
layers of the gas with the electrodes is necessary. The current
ds flow is closed by the displacement current, which is
∼ ∂ E/∂t according to Maxwell’s laws.
Alternatively, the metallic electrodes can be placed
c) in direct contact with the gas volume (Fig. 11.127b). In
IRF this case the surface regions on both electrode bound-
Coil aries have reduced free-electron densities and are called
Insulator ion sheaths. In these ion sheaths no efficient excitation
E of vibrational states takes place. Power dissipated in the
B Discharge sheaths does not contribute to the laser power. The width
of the sheaths ds is inversely proportional to the excita-
tion frequency ds ∼ 1/ f and is, for example, 0.35 mm
at f = 125 MHz at a pressure of p = 90 hPa [11.1398].
The electrode separation must be significantly larger
than this value to ensure sufficient excitation of the gas
Fig. 11.127a–c Geometries for RF excitation with current IRF and volume. On the other hand, this reduces the efficiency
electric field E: (a) capacitively coupled RF discharge, insulated of diffusion cooling for heat removal from the gas to the
electrode, (b) capacitively coupled RF discharge, non-insulated electrodes. For small gaps and efficient cooling, excita-
electrodes, (c) inductively coupled RF discharge tion frequencies in the 100 MHz range are often chosen.
Lasers and Coherent Light Sources 11.4 The CO2 Laser 739

An optimized value for the electrode separation d is no material sputtering from the cathode or anode and
typically 2 mm under these conditions. no resulting contamination of the laser gas or degra-
With insulated electrodes a so-called dielectric bar- dation by material ablation. Very high energy densities
rier discharge has been reported, which allows efficient can be applied to the gas volume while still maintain-
excitation at much lower frequencies around 1 MHz ing a stable glow discharge without arcing. Higher gas
while still maintaining a stable discharge with effi- pressures can be used, typically around 100 hPa. Thus,
cient vibrational excitation and good cooling of the more active medium and more laser power is available

Part C 11.4
gas [11.1400]. per volume. The required voltages are lower than for DC
The α-type RF discharge is a volume discharge with excitation. Insulation of electric wires and components
all ionizing and electron-collision processes taking place on the air-pressure side is easily done by sufficient large
throughout the entire gas volume. No ionizing processes air gaps or common dielectrics. The impedance of the
at the electrodes are required. Such RF discharges are gas discharge, which can be modeled as a strongly lossy
hence called electrodeless discharges. However, in the capacitor [11.1401], can be matched to the RF genera-
case of non-isolated electrodes (Fig. 11.127b) there is tor impedance with almost lossless reactive components
also an onset of a γ -type discharge at higher current (LC matching circuit). No ohmic ballast resistors are
densities, where surface ionizing processes play an im- required to stabilize the discharge.
portant role [11.1350]. This is usually not the desired However, there are also some issues to be properly
discharge type for laser excitation. considered in the design of RF-excited lasers. One of
RF gas discharges can also be inductively cou- those is voltage and discharge homogeneity along the
pled (Fig. 11.127c). The RF current IRF through a coil RF electrodes. At a frequency of 100 MHz the vac-
generates a time-varying magnetic field B which is uum wavelength λ0 is 3 m. Wave propagation effects
accompanied by an electric field E according to and waveguide theory must be applied if structures
curl E = −∂ B/∂t. Inductively coupled discharges are with one dimension  larger than λ0 /10 are used. This
not commonly used for CO2 lasers because the gas cool- is often the case for the length of typical RF-excited
ing and electrical field geometry are not as favorable as waveguide lasers. Therefore, regularly spaced inductors
for CCRFs. parallel to the electrodes are used [11.1369,1402,1403].
RF-excited discharges have several advantages. One Figure 11.128 shows an example for an electric cir-
advantage is that such an electrodeless discharge shows cuit model of the electrodes with a gas discharge.

URF (z)
Umax
Umin

z
l1 l2 l3 l4
L1 L2 L3

1 Zl , ã 2 Zl , ã 3 Zl , ã 4 Zl , ã

Impedance matching
RF feed point

Uf Z0 = 50 Ù RF generator

Zlaser Z0

Fig. 11.128 Homogenization of the RF voltage distribution URF (z) on long electrodes with parallel inductors [11.1399]
740 Part C Coherent and Incoherent Light Sources

The electrical wave propagation along the electrodes additional power for cathode heating. The lifetime of
is described by a characteristic impedance Z  and the such tubes is on the order of 10 000 hours. However,
propagation constant of a lossy transmission line γ . costs for replacement tubes are moderate.
Parallel inductors L i are used to compensate for the Finally, issues of electromagnetic compatibility
capacity per unit length of the electrodes to homogenize (EMC) have to be considered. Therefore, many RF-
the voltage distribution. The higher the RF frequency, excited lasers operate in the ISM (Industrial Scientific
the more inductors in a shorter distance li must be and Medical) bands of 13.6 MHz, 27 MHz or 40.6 MHz,
Part C 11.4

used. Also shown is an impedance-matching network where less-stringent regulations apply. Systems at differ-
to match the complex impedance of the laser Z laser ent frequencies, especially in the frequency-modulated
to the system impedance Z 0 of 50 Ω of common RF (FM) radio bands around 100 MHz need to have prop-
generators. erly shielded housings, best made of all metal and with
Alternatively, an array of segmented electrodes contact strips for all service flaps of the laser housing.
much smaller than the wavelength can be used. This Microwave excitation at a frequency of 2.45 GHz
can be problematic if the electrodes also act as wave- has been studied intensively [11.1404–1406]. Power-
guides for the laser light. Mechanical misalignment of ful magnetrons are very efficient microwave-generating
the electrode segments may then cause excessive optical tubes at this frequency and are available at low cost,
losses. because of their use in mass-produced products such
RF power generators are somewhat more com- as kitchen microwave ovens. However, the short wave-
plex than DC high-voltage supplies. They must length makes it difficult to realize large-area discharges
provide roughly ten times the nominal laser power with good uniformity. Additionally, the power density
as electrical power at RF frequencies. For low- and required to maintain a microwave-excited gas discharge
medium-power CO2 lasers up to 500 W, solid-state is larger than at common RF frequencies and tends to
RF power generators based on semiconductor tran- overheat the gas. Thus, microwave-excited CO2 lasers
sistors [mostly metal–oxide–semiconductor field-effect have been realized mostly in pulsed operation [11.1407]
transistors (MOSFETs)] are available at the required fre- or with a fast gas flow [11.1408]. Diffusion-cooled
quencies. Such RF generators can be integrated directly laser systems have also been demonstrated [11.1409].
into the laser system housing with air or water cooling In spite of the cost advantages of microwave gener-
of the power supply. ation with magnetrons, the mentioned disadvantages
For an RF power beyond this level electron-tube- and the progress of RF-excited lasers has hindered the
based generators are required. Coaxial power tetrodes, commercial success of microwave excitation to date.
as installed in amplitude-modulation (AM) short-wave
radio transmitter stations, are used. This is a mature Waveguide Lasers
and reliable technique to generate RF powers of tens For the laser design in Fig. 11.117 it would be desir-
of kilowatts in the desired frequency range. Tubes can able to reduce the diameter of the glass tube to achieve
tolerate large reflected power levels from badly matched better cooling of the laser gas. This can introduce exces-
loads without permanent damage. Electron tubes are sive optical losses by obstructing the laser beam inside
more robust against overvoltage and current transients the resonator. Losses from such limiting apertures with
than transistors. A drawback is that the tubes itself need a radius of a for common Gaussian TEM modes in
a high-voltage DC power supply and that they dissipate two-mirror stable resonators of length l are calculated

a) b) c)
IRF
IRF Metall IRF

Laser gas
Beam axis Fig. 11.129a–c Cross sections of
Dielectric some waveguides for CO2 lasers
with RF electrodes: (a) circular di-
electric waveguide, (b) all-dielectric
rectangular waveguide, (c) hybrid
metal–dielectric waveguide
Lasers and Coherent Light Sources 11.4 The CO2 Laser 741

in [11.1410]. These losses rise quickly if the Fresnel


number N = a2 /λl gets smaller than 1. Spiral inductors RF power supply
This problem can be overcome if the gas tube has Gas ballast
waveguide properties at the optical laser frequency. region
A comprehensive overview of waveguide laser design Hot electrode
is given in [11.1402]. Figure 11.129 shows the princi- Ceramic

ple geometries of waveguides used in CO2 lasers. The Plasma Al hermetically


sealed housing

Part C 11.4
simplest form is a circular hollow dielectric waveguide, discharge in
waveguides
which is theoretically described in [11.1411]. Circular
metallic waveguides are not an option because they will Cooling channels Al cooling plate
obviously shorten any electrical field required for the
discharge excitation. Rectangular waveguides can have Fig. 11.130 Cross section of a commercial RF excited waveguide
dielectric walls on all four sides or one pair of dielec- laser with a folded resonator light path
tric and one pair of metallic walls [11.1412,1413]. Such
waveguides support hybrid EHmn modes at optical fre- a ceramic plate and an aluminum profile. This results
quencies with very low losses. These modes can be in a compact laser head design with high power, as the
thought of as a superposition of electromagnetic waves laser power scales with the length of the waveguide. The
propagating at different angles to the waveguide axis, aluminum profile serves as the RF ground electrode, as
reflected by the walls at grazing incidence. Therefore, one side of the optical waveguide, as a cooling plate
the materials used should have low absorption losses in and as an RF- and gas-tight housing for sealed opera-
the infrared. Alumina or beryllium oxide ceramics are tion. The second RF electrode is on top of the ceramic
a good choice for the dielectrics because of their high plate. Regularly spaced spiral inductors homogenize the
mechanical, chemical and thermal stability and their RF voltage distribution along the structure. Air or wa-
high thermal conductivity for heat removal. Aluminum ter cooling can be realized by the cooling channels on
or gold-plated copper surfaces can be used as metallic the profile. An output power of 100 W is available from
waveguide boundaries. a compact package size [11.1417]. Q-switching can op-
The lowest circular mode EH11 is very similar to the tionally be applied to realize pulsed lasers with high
Gaussian free-space mode TEM00 , with a power overlap peak power, especially for marking applications.
of 98%. Thus, waveguide lasers operating only in the Another interesting waveguide laser structure is
lowest possible mode have excellent beam quality. shown in Fig. 11.131 [11.1418]. The waveguide is
To build a waveguide laser, such waveguides are formed by two pairs of metallic aluminum electrodes
filled with laser gas. The excitation of the gas discharge and two ridges from the metallic housing profile. RF
is therefore often realized by a transversal RF discharge. power is applied to both electrodes in a push–pull mode
A pair of metallic electrodes are placed on opposite
sides of the dielectric waveguide (Figure 11.129a,b) or Housing Ridge
are part of the waveguide itself (Figure 11.129c). The
optical resonator is realized by mirrors at both ends Insulators
of the waveguide. Design rules for low-loss coupling
and good mode discrimination are given in [11.1414]. Fins Gap
A good solution is a mirror in a small distance d from
the waveguide, which is half the radius of curvature ρ M Electrode 1 Electrode 2
of the mirror. Alternatively, plane mirrors close to the
waveguide can be used.
The power of a waveguide laser scales almost lin-
early with the length. Up to 110 W of laser power per
Discharge
meter length have been reported [11.1415].
Many commercial CO2 lasers use waveguide tech-
nology. Figure 11.130 shows the cross section of
a particular commercial waveguide laser [11.1416]. The RF power supply
resonator light path is folded in a zigzag shape three
times through multiple waveguide channels formed by Fig. 11.131 Cross section of an all-metal waveguide laser
742 Part C Coherent and Incoherent Light Sources

with respect to the grounded housing. That means that large-area metallic electrodes separated by a small gap.
the RF voltage amplitude on both electrodes is the same The length of the electrodes can be 1 m with a width of
but with a 180◦ phase shift relative to one other. The some tens of centimeters. A typical gap height is 2 mm.
electrodes are separated from the ridges by small gaps An RF voltage at a frequency in the range of 100 MHz
which enable gas circulation in the whole structure for is applied between the electrodes to start a gas discharge
cooling and heat removal. The electrodes are anodized in the laser gas mixture between the electrodes. The
such that the oxide layer provides sufficient insulation electrodes are provided with channels for cooling water.
Part C 11.4

to the grounded ridges of the housing. Additional in- Thermal energy dissipated in the gas discharge is effec-
sulators are used to hold the electrodes in the housing. tively removed by conductive or diffusion cooling. Gas
A homogeneous gas discharge is formed in the middle discharges with very large areas can be operated stably
of the structure with lateral dimensions of a few mm. In with this geometry.
spite of the small gaps, the structure can act as an opti- In a plane perpendicular to the large-area surfaces
cal waveguide in all directions to form a laser beam with the electrode pair acts as a waveguide for optical fre-
good beam quality. quencies. A low-order mode is easily obtained in this
The advantage of this all-metal structure is that waveguide direction. In the plane parallel to the elec-
no ceramic–metal joints are required. Such joints can trode surfaces free-space conditions are valid as there
potentially cause failure because of the mismatched ther- are no limiting boundaries on the sides of the elec-
mal expansion coefficients. Both the electrodes and the trodes. With such broad dimensions this would result
housing can economically be manufactured by extruded in a strongly multimode beam profile in this direction, if
aluminum profiles. Heat is easily removed by conduction common stable resonators were applied. Therefore, an
or passive thermal convection. Without ceramics with unstable resonator is used which has advantages for the
their high dielectric constants between the electrodes, extraction of high-quality beams from active laser me-
the capacitive loading of the electrical waveguide is low. dia with large transversal dimensions [11.1348, 1426].
Fewer inductors are thus required for voltage homoge- An unstable resonator is characterized by two mirrors
nization. The metal housing can be sealed with metal with radii of curvature ρ1 and ρ2 and a mirror separa-
brazing to build long-living sealed-off lasers. A range tion L that do noes fulfill the stability criterion for stable
of medium-power compact lasers up to 240 W is avail- Gaussian beam resonators:
able in this technology [11.1420], partially using folded   
L L
resonators for power scaling with the waveguide length. 0 ≤ 1− 1− ≤1 (11.140)
ρ1 ρ2
The Slab Laser Such a resonator does not reflect a Gaussian beam
Figure 11.132 shows the structure of an RF-excited backwards into itself but rather uses the partial trans-
slab laser. This design has been pioneered by several mission of the beam on one mirror side as the
groups [11.1421–1424], accompanied by the well- output coupling. It can be shown that the beam
known Tulip patent [11.1425]. It is formed by two profile can have an almost diffraction-limited beam
quality in the unstable-resonator plane. In the wave-
guide plane, the mirrors can be almost flat. Both
Cooling water
mirrors can be made of solid copper and can
Rear mirror
RF power be cooled to withstand very high power densities.
Cooling water By a proper design, the coupling losses between
the mirrors and the slab waveguide can be mini-
Output coupler
mized [11.1427].
Discharge The laser beam coming directly from this type of
Beam forming resonator has an elliptical shape and has different diver-
Electrodes
gence angles in the waveguide and the free-space plane.
Laser beam This is corrected by beam-shaping optics with at least
one cylindrical mirror. Additionally, a spatial mode fil-
ter is used to eliminate shadows on the beam wings in
the free-space unstable-resonator direction. After that,
Fig. 11.132 RF-excited slab laser with hybrid waveguide-unstable the beam has a nearly circular shape with an excellent
resonator [11.1419] beam quality of M 2 = 1.1.
Lasers and Coherent Light Sources 11.4 The CO2 Laser 743

The main advantage of this structure is that the laser


Turbo radial blower
power can be scaled by the area Ae of the gas discharge, Pre-cooler
Gas flow
which extends in two dimensions. This is in contrast to
Heat exchanger
tube-type or waveguide lasers where the power scales
only over one dimension, namely the tube length L.
From thermodynamic calculations and based on ex-
tending results from conventional waveguide lasers, the

Part C 11.4
maximum laser power PL of a slab with an electrode
area Ae and an electrode separation de is approximately
given by: Bending
mirror
Ae W mm
PL = C , C≈3 . (11.141) Discharge
de cm2 Glass tube Rear mirror
By this area scaling over Ae , very compact and yet pow- RF electrodes Laser beam Output coupler
erful lasers can be made. As with all large RF-excited
laser systems, parallel inductors are used for homo- Fig. 11.133 RF-excited fast axial gas flow with a folded res-
geneous RF voltage distribution along the electrodes. onator [11.1428]
The efficient diffusion cooling requires no gas flow,
which saves system and operating costs. Medium-power system. Volume flow rates are up to 500 m3 /h per kW
lasers can be operated completely sealed and are avail- extracted laser power with gas velocities of 100 m/s.
able at power levels up to 500 W [11.1429], partially Lasers with output powers up to 20 kW are commer-
with transistor-based RF generators. High-power slab cially available while laser powers above 30 kW have
lasers operate typically with a periodic gas exchange, been demonstrated experimentally [11.1430]. The beam
for example after 72 h of continuous operation, to com- quality is near a perfect diffraction-limited TEM00 mode
pensate for residual gas leaks from the large structure. with an M 2 of 1.1 for high-quality series up to 4 kW.
Commercial slab lasers with powers up to 8 kW in- At the high-power end the 20 kW system still has an
tegrate the slab structure and the electron-tube-based M 2 value as low as 5. The wall-plug efficiency of these
self-oscillating RF generator into one compact housing systems is 10% including the losses in the RF power sup-
with an integrated premix gas supply which lasts for ply and the gas-circulating system. Electron-tube-based
approximately 12 months of continuous use [11.1419]. high-power RF oscillators at an industrial ISM standard
frequency of 13.6 MHz are used.
RF-Excited Fast-Flow CO2 Lasers
The basic principle of a fast-axial-gas-flow laser as Other RF-Excited CO2 Laser Systems
described in Sect. 11.4.2 can be combined with the ad- There are many other commercial laser designs based
vantages of RF excitation. Figure 11.133 shows such on RF excitation and with specific resonator or cooling
a laser system. The gas circulates through glass tubes geometries. Some interesting designs will be discussed
driven by a turbo radial blower in the center of the struc- briefly here.
ture. The optical resonator is quadratically folded. For an
even longer discharge length and more output power, the
resonator can be folded in two planes with 16 discharge 1
sections (Fig. 11.134). Optically stable resonator con-
figurations are used. The RF discharge is capacitively
1
coupled with eight pairs of electrodes, two on each side.
The electrodes are mutually rotated by an angle of 45◦ 2
to ensure a homogeneous gain in the cross section, aver-
aged over one resonator cycle. A heat exchanger cools 4 4 3
the gas coming from the discharge section and a pre-
1 Bending mirrors 3 Output coupler
cooler removes compression heat after the blower before 2 Rear mirror 4 Gas discharge tubes
the gas enters the discharge sections again. Typical gas
pressures are in the range of 150 hPa. The power scaling Fig. 11.134 Quadratically folded resonator in two planes
with mass flow according to (11.139) is also valid for this [11.1428]
744 Part C Coherent and Incoherent Light Sources

free-space plane again. Sealed-off OEM modules in an


Spherical rear mirror
all-metal design and a maximum power of 400 W can
be realized [11.1435].
Three-times folded resonator Large-area RF-excited gas discharges can also be
combined with a fast gas flow between the electrode
plates transversally to the optical resonator and the laser
Electrode beam (Fig. 11.136). The gas flow is driven by a tangential
Part C 11.4

Beam on blower integrated into the large-diameter cylindrical gas


Plane total reflector rear mirror vessel. A folded resonator is used to extract the energy
Output coupler Electrode from the large active medium. Such lasers can produce
8 kW of laser power from a very compact footprint. The
Fig. 11.135 Folded free-space resonator between large-area slab beam quality with M 2 ≈ 5 is still well suited for welding
electrodes [11.1431] and surface-treatment applications.
Coaxial laser systems with an annular gas discharge
Figure 11.135 shows a folded free-space resonator as shown in Fig. 11.137 can be thought of as slab-type
between two large-area RF electrodes. Only three mir- lasers with an electrode pair rolled up to form coax-
rors are required for beam folding. The output coupler ial tubes [11.1436]. RF power is applied to the inner
and the plane total reflector can even be integrated tube, while the outer tube is grounded. This is similar
in one mirror with inhomogeneously reflecting coat- to a coaxial cable, but with an inner-conductor diameter
ings. Compact and robust sealed original equipment of approximately 10 cm and a discharge gap width of
manufacturer (OEM) laser modules up to 120 W are 7 mm, for example. In this design, the electrodes have
available [11.1431]. no optical waveguiding properties, thus such lasers are
A combination of large-area electrodes with a hy- less susceptible to power and beam-quality variations
brid stable–unstable resonator is described in [11.1433] under mechanical and thermal stress. The resonator is
and [11.1434]. In contrast to the slab laser with its formed by a helical mirror and an axicon mirror, bending
plane-parallel electrodes, the electrodes do not act as the beam to the opposite side of the tube while slightly
a waveguide here. Instead, they have a slightly V- shifting the azimuthal angle after each pass [11.1437].
shaped surface geometry along the beam propagation In the radial direction the optical resonator configu-
direction between the mirrors to select the lowest-order ration is stable, while in the azimuthal direction an
free-space mode in a plane perpendicular to the elec- unstable resonator is used. The laser is diffusion-cooled
trodes, whereas an unstable resonator is used in the by water-cooled electrode tubes. The laser can be op-
erated quasi-sealed-off with a regularly scheduled gas
exchange. Compact and robust lasers with 2 kW power
Heat Real time can be realized [11.1438]. They are well suited for
exchanger power monitor
Gas flow mounting on moving systems such as robots without
direction
bending mirrors for beam steering.
Tangential
blower Pulsed TEA Lasers
Rear
mirror All the laser designs discussed so far are continuous-
wave (CW) lasers by principle. Their power can be
modulated by the electrical excitation power with fre-
Fold mirror
quencies of a few kHz for DC excitation and up to
100 kHz for some RF-excited lasers. In contrast, the
RF electrodes tranversal-excited atmospheric-pressure (TEA) laser is
a CO2 laser that can inherently operate only in pulsed
Fold mirror mode, but is capable of generation very high pulse en-
Laser beam
Output mirror
ergies and peak powers that are not possible with CW
Output window
CO2 lasers. This is achieved by a high gas pressure, at
atmospheric pressure or above. A homogeneous DC dis-
Fig. 11.136 RF-excited laser with fast transversal gas charge can only be operated for a short time of 1 µs under
flow [11.1432] these conditions before filamentation and arcing would
Lasers and Coherent Light Sources 11.4 The CO2 Laser 745

start. The required voltages at this pressure are in the


Axicon mirror
order of magnitude of 100 kV per meter. Longitudinal
discharges would need voltages that are not practical and
would not produce stable discharges. Therefore, pulsed Helical mirror
transversal discharges are used. Figure 11.138 shows
a sketch of a simple TEA laser circuit. A high-voltage
power supply (HV) charges a storage capacitor C slowly

Part C 11.4
via the resistors RV 1 and RV 2 . When the maximum volt-
age at the capacitor is reached, a fast high-voltage switch,
which is also capable of carrying high currents, is trig- Inner tube, electrode
gered to close the circuit quickly. The capacitor voltage Annular gas discharge
Outer tube, electrode
is applied to the electrode pair, where a short but intense
discharge transversal to the resonator axis and the laser ZnSe window
beam starts. The discharge self-terminates when all the Fig. 11.137 Coaxial laser with an annular gas discharge [11.1439]
energy stored in the capacitor is dissipated. Afterwards
the high-voltage switch resets itself to an open state and
charging of the capacitor starts again before the next Wavelength Selection and Tunable CO2 Lasers
pulse can be triggered. Without any wavelength-selective elements, a CO2 laser
With TEA lasers pulse energies in the range of emits at wavelengths around 10.6 µm in the vicinity of
10 J per liter of active volume and per bar of pres- the 10P(20) line. Some commercial lasers are optionally
sure can be achieved, with peak intensities in the MW available at the wavelengths of the strongest lines of the
range [11.1440, 1441]. Pulse repetition rates are a few other bands, for example at 9.3 µm, 9.6 µm or 10.3 µm
10 Hz for high-power systems and kHz for mini-TEA (Fig. 11.122). This is done by weakly wavelength-
lasers [11.1442]. selective elements such as mirror coatings to select one
Critical design issues are the electrode profile to of the four regular emission bands where the strongest
maintain a stable and homogeneous discharge in the line will start to oscillate. For example, this is interest-
cross section and also over the length of the elec- ing for plastics machining where materials can show
trodes. Often pre-ionization techniques by additional a strong variation of absorption over wavelength.
electrodes, UV light from corona discharges or even For precise selection of a particular roto-vibrational
electron beams are therefore applied. The high-voltage transition, a diffraction grating is used. Figure 11.139
switch is also a crucial part. Typically, triggered spark shows a DC-excited tunable laser in the Littrow config-
gaps or thyratrons are used, which must be replaced uration. Depending on the angle α of the incoming beam
after a given number of pulses. Recently, progress with respect to the surface normal of the grating, only
in semiconductor technology has made it possible to a light beam at a specific wavelength λL is reflected:
replace these vacuum tubes by solid-state switches.
λL = 2Λ sin α , (11.142)
A device called a silicon controlled rectifier (SCR) is
capable of switching high currents very fast. In com- with Λ being the grating period. For this particular wave-
bination with a step-up transformer and a saturable length λL the grating acts as a plane reflector on axis to
inductor/capacitor ladder network the high-voltage level the second resonator mirror. This wavelength is selected
and the fast rise time required for the electrode voltage
can be achieved.
Much research was done on TEA lasers in the
C Electrode
1980s, especially in the fields of plasma physics, LIDAR
and military applications. Partially due to the suc- RV1
cess of high-power fast-flow and RF-excited systems, Discharge
only a few commercial TEA lasers are available. Sys- Trigger Beam axis
tems with pulse energies of 2.4 J at a repetition rate HV RV2
of 125 Hz are available, for example. Applications in- Switch Electrode
clude non-metal processing such as marking and paint
or rubber-compound stripping from surfaces in the au-
tomotive industry [11.1443]. Fig. 11.138 Excitation circuit for a basic TEA laser
746 Part C Coherent and Incoherent Light Sources

Fig. 11.139 Tunable CO2 laser in


Spherical output Littrow configuration
coupler UDC Brewster
plate
Beam ëL á

Ä
Discharge tube ëx
Diffraction grating
Part C 11.5

Table 11.41 Emission range of a tunable CO2 laser [11.1444]


Band Wavelengths (µm) Lines
min – center – max min – center – max
9R 9.158 – 9.271 – 9.367 9R(44) – 9R(20) – 9R(4)
9P 9.443 – 9.552 – 9.836 9P(6) – 9P(20) – 9P(50)
10R 10.095 – 10.247 – 10.365 10R(46) – 10R(20) – 10R(4)
10P 10.441 – 10.591 – 10.936 10P(4) – 10P(20) – 10R(50)

to lase. Other wavelengths λx , if present, would be re- Applications include scientific spectroscopy, indus-
flected at a different angle not parallel to the resonator trial trace-gas monitoring by absorption spectroscopy or
axis. They would suffer significant losses from the aper- optically pumping of far-infrared molecular gas lasers.
ture of the laser tube, which would prevent them from By using gas mixtures enriched with special isotopo-
lasing. By rotation of the grating the angle α can be var- logues, for example 13 CO2 , emission lines at additional
ied to select different roto-vibrational transitions one by wavelengths can be realized. Tables of such wavelengths
one. Such gratings are mostly made of copper or steel are given, for example, in [11.1347].
with precision-ruled grooves and a gold coating to en- Besides longitudinally DC-excited lasers, RF-
hance IR reflectivity. The grating period Λ is chosen to excited waveguide lasers are also good candidates
be slightly smaller than the laser wavelength in order to for being tuned by a standard Littrow grating. Tun-
suppress higher diffraction orders. The groove geometry able slab-type lasers with their broad active medium
can be adjusted such that the reflectivity in the desired require special grating structures for the extrac-
minus-first diffraction order at a given wavelength is tion of a low-order mode. This can be realized
maximal (blazed gratings, blazing wavelength). by apodized Littrow gratings where the splitting
Table 11.41 shows for example the tuning range of ratio between the diffraction orders m = 0 and
a commercial tunable CO2 laser. Note that, because of m = −1 is variable over direction of the grat-
the separation of the rotational lines in the range of ing [11.1445]. Such gratings can act as an output
30–90 GHz and the pressure-broadened line width of coupler with spatially variably reflectivity for beam
some 100 MHz, continuous tuning over the entire range forming and as line-selective element for wavelength
is not possible. Within one line width, fine-tuning can be tuning at the same time. They have been realized
done by changing the resonator length with a piezoelec- on copper mirror substrates with photolithography
tric element. An output power of 180 W can be achieved and a microgalvanic process as well as on silicon
for the strongest lines and more than 20 W on the weak substrates with photolithography and anisotropic etch-
lines at the band edges, for example. ing [11.1446].

11.5 Ion Lasers


Ion lasers became a success very soon after their tion, and medical technology. Mid-power ion lasers
invention in the 1960s. In the following decades, were a staple of the entertainment industry, used in
low-power air-cooled argon lasers were made in the light shows, special effects, and for holography, as
tens of thousands for use in printing, color separa- well as in disc mastering. Large-frame ion lasers
Lasers and Coherent Light Sources 11.5 Ion Lasers 747

were ubiquitous in well-equipped chemistry and bi- A high-performance ion system has a laser head
ology laboratories around the world. Ion lasers were about a meter and half long and can weigh 100 kg. It
the flagship products of the major commercial laser may require 70 A per phase of three-phase electrical
manufacturers. service at 480 V and in addition a cooling-water flow
But even in their heyday, alternatives to ion lasers of several liters per minute. But in compensation, these
were eagerly sought. There were several reasons for this, lasers are capable of producing many watts of continu-
including early problems with reliability and lifetime, as ous laser power in a range of selectable wavelengths not

Part C 11.5
well as high cost, but the major dissatisfactions resulted available from any other commercial laser system.
from the fundamental low efficiency of the devices. This Wavelengths available from ion lasers extend from
poor efficiency meant ion lasers were large, of consid- the infrared well into the ultraviolet, with argon, the most
erable weight, and needed substantial power supplies common type of ion laser, emitting light primarily in the
drawing large utility loads. They also had to be cooled blue–green to ultraviolet range [11.1447,1448]. Specific
aggressively either by air or water. wavelength output is determined either by the choice of
With the development of solid-state lasers in the coating for the laser output mirror, or by tuning to the
the 1990s, in particular diode-pumped lasers with desired wavelength using a Littrow prism placed in the
frequency-doubled green output at 532 nm, many ex- laser resonator. The section below discussing the laser
pected ion-laser technology to become obsolete. This resonator will further describe control of the spectral
has not happened. While not nearly at the levels they characteristics of the ion-laser output.
experienced in the 1980s, sales continue to be steady, Krypton is not nearly as popular an ion laser as ar-
ion lasers are still found in their traditional applications, gon, in part because of its lower power, but it remains
and are a significant contributor to the bottom line of commercially viable because, like argon, it offers signif-
a number of companies, both as new systems and in the icant levels of continuous output power at wavelengths
replacement market. While there are fewer types of new not easily achieved by other means. For example, more
ion lasers available now, these systems still vary con- than 1 W CW is available from a single line in the yellow,
siderably in performance, size, utility requirements, and a color region where laser sources are scarce, and lines
cost. in the violet and ultraviolet have important applications
An ion-laser system consists of a power supply, con- as well.
trol electronics, and the laser head. The laser head itself The output power of an ion laser depends on two
contains the plasma tube placed within a resonator (or sets of variables. One set derives from the design of the
cavity) structure. Control of the laser is typically through laser resonator, and includes, for example, the cross-
an interface included in the power supply, which itself sectional area of the laser beam. This set of variables
can vary considerably in size, complexity, and cooling will be discussed in the section which describes the res-
requirements. onator. The other set of variables that determines laser
Small ion lasers are air cooled, require only standard power results from the physics of the laser process in
wall-plug electrical service, have a laser head roughly the plasma created from the noble gas. These variables
the size of a toaster, and are most commonly used to include the total light amplification available from the
produce only a single blue–green output at 488 nm in plasma.
the range 5–100 mW. When operated in the low-current
range, these lasers can be expected to last for years in 11.5.1 Ion-Laser Physics
a stable environment. Tube replacement when necessary
can be performed by the user and is relatively quick and An energy-level diagram is used to show the wave-
inexpensive. lengths available from a laser material that has been
The greatest variety of product offerings is in the excited into a condition of population inversion. A sim-
mid-range of performance of 1–5 W of laser out- plified version illustrating the transitions in singly
put. These systems range from simpler models based ionized argon that produce visible laser light is shown
on the original ion technology, with air cooling and in Fig. 11.140 [11.1449]. The transitions shown result
ceramic plasma tubes, to specialized systems with from energetic electrons that have decayed to the 4p up-
single-wavelength output intended for specific indus- per laser level from a still higher level not shown in
trial applications, to only slightly smaller versions of the figure. From the upper laser level, the electrons are
the sophisticated large-frame systems used in advanced stimulated to fall into the 4s states. The most important
laboratories. individual transitions, which result in the highest output
748 Part C Coherent and Incoherent Light Sources

1/2 4p2S0
3/2
1/2 4p2P0
465.8
3/2
5/2
4p2D0
457.9 4p
488.0
476.5
472.7 1/2
Visible
» 2 eV laser » 20 eV Pumping
Part C 11.5

3/2
transition transition
496.5 4p4D0
5/2
454.5 528.7 7/2
4s

1/2 514.5
4s2P
3/2

3 p5 Ar +
Fig. 11.140 The visible laser transitions of ionized argon
(wavelengths in nanometers)
Ionizing
»16 eV transition
power, are those for 488.0 nm, a blue–green color, and
514.5 nm in the green.
3 p6 Ar
Having many upper laser levels transitioning to only Neutral argon ground state
two lower levels raises the possibility of competition
for the lower states, which can limit laser output. In Fig. 11.141 The two-step ion-laser excitation. One electron
the case of argon, however, the lower states depopulate collision ionizes neutral argon and a second pumps the ion
to the ground state very rapidly, avoiding this potential to an excited state from which it decays to the upper laser
bottleneck. The lifetime of an electron in one of the level
upper 4p states is about 10 ns, while the lower 4s states
make their transition to the ground state in a favorable argon ion to the upper level of visible lasing transitions.
0.5 ns. With a proper choice of mirror coating, all-lines The gain available from the ionized gas therefore varies
visible operation can produce laser power from most of as the square of the current density, up to the point where
these visible lines simultaneously, and the power present the gain saturates (i. e., other gas-phase processes begin
in any one of the lines will not be much less than that to limit the gain) [11.1451].
obtained from single-line operation. The optimum gas pressure that produces the max-
An energy-level diagram can also illustrate prob- imum laser output is a balance between competing
lems or requirements in the design of a specific laser factors. High pressure provides a greater number of
system. Figure 11.141 shows the 4p and 4s laser lev- potential ions to stimulate laser emission, while low
els of ionized singly argon in relation to the argon pressure allows the voltage drop along the plasma more
ground state. The energy needed to ionize the argon time to accelerate the free electrons to a greater energy
to start the population inversion is about 16 eV, and between collisions. Different wavelengths have differ-
an additional 20 eV is required to reach the states that ent optimum pressures, and the final choice for a laser
decay to the upper laser level. Comparing this total en- designed to operate at multiple wavelengths is a com-
ergy input of 36 eV to the energy emitted by the laser promise. In general the optimum is in the low-pressure
transition itself, about 2 eV, it is evident that the effi- regime. Argon plasma tubes have a fill pressure on the
ciency of an argon ion laser will be low. In addition, order of 1 Torr [11.1452].
the temperature of the gas discharge needed to produce Performance is improved by a magnetic field di-
electrons with sufficient kinetic energy to achieve the rected along the length of the plasma discharge, which
required level of ionization is in the vicinity of 3000 K. helps confine the discharge towards the center of the
This, combined with the low efficiency, indicates that plasma tube [11.1450]. The benefit is greatest for lasers
heat management is a primary concern in ion-laser operating at high current. Again, different wavelengths
design [11.1450]. have different optima, and a compromise value of
Ion lasers use an electric discharge to energize the magnetic field strength is employed. Air-cooled lasers
gas. As can be seen in Fig. 11.141, two collisions with typically do not use magnets, as the benefit of a magnetic
free electrons are required to excite an electron in an field for low powers does not justify the added expense,
Lasers and Coherent Light Sources 11.5 Ion Lasers 749

and the addition of magnets would complicate the flow the component wavelengths change in relative strength
of cooling air. of output.
If the argon is doubly ionized (i. e., stripped of two
electrons), a new set of transitions become available that 11.5.2 Plasma Tube Design
produce ultraviolet laser light [11.1453]. The ground
state of Ar2+ is about 43 eV above that of the neutral The heart of the ion laser is the plasma tube, which am-
atom, compared to the Ar+ ground-state difference of plifies laser wavelengths available from a low-pressure

Part C 11.5
16 eV mentioned, so operating in the ultraviolet can be noble gas by confining a high-current discharge within
expected to be even less efficient. Once above a higher a narrow bore. The demands placed on the tube struc-
threshold current, UV output rises more rapidly than the ture are extreme, resulting from the need to confine and
visible output does. sustain a discharge as high as 70 A for hours at a time.
The energy diagram for krypton is similar to that The bore of the tube must withstand the bombardment
for argon, with laser transitions shifted to somewhat of high-energy ions (sputtering) and the heat from the
lower photon energies in the visible from the upper discharge, which can exceed 50 kW under some oper-
5p to the lower 5s bands [11.1454]. Important lines ating conditions. This heat must be efficiently removed
are at 647.1 nm in the red, corresponding to the green from the tube or tube components will melt or rupture.
514.5 nm argon line, and at 568.2 nm in the yellow, cor- Early tube designs relied on cylinders of the ce-
responding to the blue–green line at 488 nm in argon. ramic beryllia, or BeO, about 1–2 cm in diameter with
Unlike argon, however, in krypton these strong lines do a centrally drilled hole of about 1 mm to form the bore.
experience competition for the same lower state, and Beryllia cylinders about 10 to 15 cm long are still in
so all-lines operation in krypton does not produce the use today in lower-power ion lasers, particularly for air-
power that might be expected judging from single-line cooled argon. Figure 11.142 shows a cross section of
output. an air-cooled plasma tube. However beryllia proved in-
Argon and krypton can be mixed together in the same capable of sufficiently withstanding the sputtering from
laser tube to produce a laser offering a dazzling variety of the plasmas of high-power or ultraviolet ion lasers, and
visible wavelengths. A compromise must be reached in alternative designs were sought.
the parameters such as fill pressure and magnetic field Years of intensive research and development have
that allows for the differences in the optimization for resulted in sophisticated designs for high-current tubes
each type of laser. Such a mixed-gas laser using broad- that replace beryllia with a tube structured of compos-
band mirror coatings has even been used to produce ite materials [11.1452, 1455]. These complex (and more
a white-light laser, but the argon–krypton mixture be- expensive) designs can withstand high current densities
comes unbalanced fairly quickly due to the difference in for an extended period, thus making practical the op-
gas sputtering rates, and the white-light balance is lost as eration of ion lasers at higher powers or less-efficient

High reflector
mirror
Deformable Gas return Bore
mirror mount path capillary

Output mirror Anode Ceramic bore Cathode


(cooling fins Polarizing Brewster
deleted for clarity) window

Fig. 11.142 Design of an air-cooled plasma tube


750 Part C Coherent and Incoherent Light Sources
Part C 11.5

1 2 3 5 6 4 7 8 9
Fig. 11.143 Design of a water-cooled plasma tube

wavelengths. The description that follows is based on The design of the cathode element itself is also crit-
the segmented-bore technology used by Spectra-Physics ical. The cathode is helical and is made from a spongy
in the manufacture of its water-cooled ion lasers. The material formed of tungsten powder. It may also in-
overall design is illustrated in Fig. 11.143. clude some admixture of calcium, aluminum, barium,
The exterior of the plasma tube is a long, hollow and strontium. These additives reduce the work function
thin-walled ceramic pipe or sleeve a few centimeters in of the cathode surface so that the temperature needed to
diameter. Inside this sleeve, spaced about one centimeter produce electron emission is reduced [11.1455].
apart, are many thin discs brazed to the interior of the The efficiency of laser amplification is a function of
ceramic. The discs are copper with a central tungsten the gas pressure in the discharge. However ionic sputter-
ring with a hole a few millimeters in diameter. The bore ing not only erodes the tube materials, but also over time
of the plasma tube is defined by the diameter of the hole embeds a significant amount of gas in the tube walls and
in the tungsten segments (Fig. 11.144). components. Low-power lasers compensate for this ef-
The tungsten bore segments are extremely resistant fect by widening the body of the plasma tube to form
to sputtering action and can withstand the high tempera- a reservoir, so that the gas lost from sputtering action is
tures of the discharge. The copper discs to which they are a small fraction of the total volume in the tube. Mid- and
bonded conduct the heat of the discharge from the tung- high-power designs incorporate an active fill system to
sten to the thin ceramic wall of the exterior sleeve, which replenish the gas as it is lost.
is bathed outside by a cooling water flow of several liters To determine when the gas must be replenished,
per minute. The flow of this cooling water is designed a microprocessor compares the operating voltage of the
to prevent local thermal stresses affecting the tube. laser to values stored in a look-up table, taking into
The plasma tube must ensure uniform gas pressure account the current, magnetic field and warm-up time.
along the length of the bore. In arc discharges in low- When the voltage indicates that the tube pressure is low,
pressure gases, the ions lose their momentum in frequent a high-pressure reservoir automatically injects a small
collisions with the tube walls. In contrast, the electrons quantity of gas into a plenum. A separate valve then
lose little momentum, so an imbalance is created in the
net momentum in the gas. As a result, the neutral gas Magnet
atoms are driven to the anode end of the plasma tube. To Water
equalize the gas pressure along the length of the tube, Ceramic
holes in the copper discs provide a return path to the envelop
cathode end, which also allows the copper discs to help Copper
cool the gas in the return flow. heat web
The design of the bore where it opens to the cath- Tungsten disk
ode, the so-called throat region, is critically important Bore
to achieve good laser lifetime. Damage to the bore from
sputtering is maximum in the throat. The diameter of the
bore segments (or, in lower-power tubes, the conically
shaped opening drilled in the beryllia to form the throat) Fig. 11.144 Seg-
is tapered to match the contour of the electrical field as mented bore
it enters the bore. design
Lasers and Coherent Light Sources 11.5 Ion Lasers 751

opens to allow the plenum to add a precise quantity of deleterious to optical materials. The coatings on the mir-
gas to the plasma tube. Since this fill process briefly rors that seal low-power and some mid-power tubes are
disturbs laser operation, the fill system may be man- made of many alternating layers of dielectric materials,
ually disabled for short periods to ensure that critical such as silica and alumina, that are capable of with-
experiments are not effected. standing this radiation. Brewster windows used to seal
For air-cooled lasers, which do not employ a mag- mid-power lasers are typically made of fused silica.
netic field, copper cooling fins are brazed onto the The levels of the vacuum ultraviolet of high-current

Part C 11.5
exterior of the beryllia cylinder that forms the plasma discharges present a greater problem for the Brewster
tube. Cooling air is forced over the fins at a rate of window seals of these tubes [11.1456,1457]. Fused silica
a few hundred cubic feet per minute (about 10 m3 per cannot be used because, when exposed to these radi-
minute). Care must be taken that heat removal is evenly ation levels, it forms color-center defects which then
distributed so that the tube does not warp and move the absorb even more radiation in a runaway effect that will
laser beam (the laser output mirror is attached directly degrade laser action. To meet the challenge of sealing
to the tube), and the air flow should not induce vibra- high-current plasma tubes, manufacturers use crystalline
tions in the fins which might translate into motion of the quartz, carefully cut and oriented on the tube so that the
beam. crystalline axis of the two windows on each end of the
For larger lasers, the entire plasma tube is encased tube are in alignment.
in a large electromagnet which also forms the confining
wall for the water flowing next to the tube. The field cho- 11.5.3 Ion-Laser Resonators
sen for the magnet depends on the diameter of the bore
and the details of how the laser is operated, but is usually To complete the ion-laser structure, the plasma tube
in the neighborhood of 1000 G. The magnetic field is par- must be placed between suitable mirrors that provide
ticularly important for ultraviolet output, which requires light feedback for amplification by the discharge. These
stronger magnetic fields for optimum performance. mirrors are a high reflector at one end of the laser,
The ends of the plasma tube are sealed with optics and a partial transmitter or output coupler that allows
that allow the laser light to exit the tube. These optics a portion of the circulating light to exit the laser. These
are either laser mirrors with dielectric coatings, used in mirrors, together with the structure that holds them in
essentially all low-power and some mid-power lasers, position, form the laser resonator [11.1458]. For small
or quartz windows oriented at Brewster’s angle. Tubes ion lasers and some mid-frame systems, this resonator
are constructed with Brewster windows to polarize their structure is very simple: the mirrors are bonded onto the
output, generally oriented vertically. Mirror-sealed tubes plasma tube itself.
will have an internal optic to achieve polarization. Air-cooled ion lasers sacrifice flexibility for sim-
The light emitted from the discharge of high-current plicity. Except for the power level, their output
tubes poses a challenge for optics. The transitions from characteristics cannot be changed. A mirror position is
the lower laser levels back to the ground state of neu- fixed at manufacture by the plastic deformation of the
tral argon shown in Fig. 11.141 emits a highly energetic thin metal tube to which the mirror is bonded. The out-
photon around 80 nm. This vacuum UV radiation is very put wavelength, mode structure of the beam, and so on

Mirror front plate Resonator Mirror end plate

Bearing Magnet with plasma tube Bushing

Fig. 11.145 Open resonator design


752 Part C Coherent and Incoherent Light Sources

remain fixed. For many applications this is acceptable, mechanical stability provided for stable power and beam
even desirable, but other applications benefit greatly by pointing [11.1459].
retaining the flexibility of output that is a hallmark of A significant advantage that modern large-frame
the ion laser. lasers have over their forerunners is the use of ac-
The external or open resonator commonly employed tive mirror positioning. The output coupler is mounted
with mid- and large-frame systems retains this flexibil- on three-point piezoelectric positioner that provides
ity. This design requires the use of Brewster-window small corrections to the mirror alignment in response
Part C 11.5

seals for the plasma tube, as discussed in the preced- to changes in laser output power, most commonly ex-
ing section. The resonator mirrors are held in place by perienced when the laser is warming up. This active
a rigid structure that frames the plasma tube (hence the resonator also allows for a more aggressive optical
use of mid-frame or large frame as an indication of design to extract power from the plasma tube.
laser size). While it outwardly appears simple, the de- With active mirror positioning, the cross-sectional
sign of the resonator is critical to the performance of the area of the beam, and therefore the volume of the plasma
laser. discharge used to provide laser amplification, can be in-
The resonator frame, as shown in Fig. 11.145, must creased by enlarging the bore and using a longer-radius
keep the mirrors aligned to each other and pointing output coupler (Fig. 11.146). This is especially benefi-
through the laser bore within a very tight tolerance over cial for wavelengths with lower gain. However active
the entire range of operating and environmental condi- control alone cannot provide all of the stability required
tions. The choice of materials affects the stability of the by this design: the use of long-radius optics requires an
resonator. The ideal material has both a low thermal ex- extremely rigid resonator structure.
pansion coefficient and a high ability to distribute heat The open resonator allows the user to employ dif-
evenly. Graphite and low-expansion compounds such as ferent mirrors to obtain different wavelength output. To
iron–nickel alloys are typically used for the long rods obtain all-lines argon-ion output in the visible, for ex-
that form the length of the frame. ample, mirrors are used with coatings that reflect over
Stability also depends on the rigidity of the res- about 70 nm in the blue and green. A prism on a rotat-
onator. Jitter impressed on the laser output due to the able mount placed before the high reflector allows the
microphonic movement of the mirrors can be caused by laser to be tuned to single-line output throughout the
cooling-water flow, vibration of the resonator structure, all-lines range. (The dispersion of the prism directs only
and acoustic noise. Isolation of the resonator from both one wavelength at a time to the high reflector.) A simi-
the plasma tube, the magnet, and the cover of the laser lar arrangement using different optics enables the same
head helps reduce jitter. operation for all-lines ultraviolet output.
The mechanical design of the structure is also critical The open resonator also allows the spatial mode of
to stability. The most stable configuration is an arrange- the beam to be controlled. An adjustable aperture placed
ment of three resonator rods in an equilateral triangle. between the Brewster window and the output coupler,
As a practical matter, this ideal structure does not leave where the beam is large, provides a variable amount of
sufficient room for the plasma tube and magnet. As one loss to the edges of the beam while it is inside the res-
of the angles of the resonator triangle increases, the re- onator. The aperture, when opened to allow the highest
sistance to flexure is reduced. The closer the design can power output, will permit a number of transverse modes,
be to the ideal equilateral triangle, the better will be the or if reduced will result in TEM00 mode operation. An
aperture diameter between 1.5 and 2 times the TEM00
mode diameter is used to achieve this [11.1460].
Spherical Additional Flat high
output coupler mode volume reflector
The spectral content of the laser output may also be
changed by insertion of an etalon into the laser resonator.
An etalon is a thin optical cavity, such as a plate of glass.
When inserted into the resonator, the internal reflections
from its surfaces act to narrow the frequency content of
the laser output, its line width. The resonator produces
Plasma Short center of Long center of standing waves of light between its mirrors, called longi-
tube bore curvature curvature
tudinal modes, many of which have frequencies that fall
Fig. 11.146 Active mirror positioning allows resonators to extract within the bandwidth of the laser amplifier. The etalon
more power from the discharge acts as a bandpass filter that introduces variable loss and
Lasers and Coherent Light Sources 11.5 Ion Lasers 753

a large-frame system in Fig. 11.148. Typically packaged


Laser gain profile in the laser head along with the plasma tube are the start
Longitudinal modes circuit and the light pick-off. Lasers that are not sold
Etalon loss as OEM components for a larger system are required to
have an interlock switch that will reliably terminate laser
operation if the head cover is opened. For water-cooled
lasers, the laser head will usually also contain the flow-

Part C 11.5
and temperature-control circuits for the cooling water,
and the fill circuitry to monitor and replenish the gas in
the plasma tube.
Output power The start circuit provides a high-voltage spark to ini-
tiate the discharge. Typically, a pulse of several kV is
injected in series with the tube by a pulse transformer or
a spark-gap circuit. The light pick-off is the sensor for
Resulting the feedback loop that measures and regulates the laser
laser output output power, and usually consists of a beam splitter
with a silicon photodetector. Since an ion laser may be
capable of producing a wide spectrum of wavelengths
Frequency
over a considerable range of powers, multiple pream-
plifier ranges are usually used in the feedback loop, as
Fig. 11.147 Using an etalon to narrow the spectrum of the well as wavelength sensitivity correction color filters or
laser output electronic gain modification.
The power supply that drives the plasma tube is
favors oscillation on only one of the longitudinal modes almost always packaged as a separate unit. This is be-
(Fig. 11.147). cause the supply itself is roughly the same volume as the
Active mirror positioning may also be used to stabi- laser head, and separating it from the laser allows much
lize the line width further, resulting in an even narrower greater flexibility in positioning the laser system. The
spectral output. The coherence length – the distance over drive current for the plasma tube is delivered to the laser
which the output beam maintains a fixed phase relation- head through a robust umbilical. Since the power supply
ship – is inversely proportional to the line width. When also serves as the control interface for the laser, cables
the laser output is changed from single line to single
frequency, the coherence length increases from about
50 mm to 20 m. Magnet
regulator
A drawback of the open resonator is that the space
between the mirrors and the Brewster windows is not
Start M
vacuum-sealed. Laser performance strongly depends on a
circuit
keeping these optical surfaces clean. In addition, the Plasma g
vacuum UV light from the arc discharge, transmitted tube n
Main e
by the Brewster windows, converts oxygen to ozone, EMI Plasma Gas fill
rectifier/ t
which is deleterious to the laser optics. This intracavity filter regulator system
filter
space must be sealed and its atmosphere controlled to
maintain cleanliness and avoid optical damage. Lasers Filament
producing short-wavelength UV may employ a nitrogen supply
Interlocks
purge to avoid ozone production. Longer-wavelength Power
lasers can use a simpler technique of placing a catalyst in monitor
the enclosed space that converts ozone back into oxygen. Operator
interface

11.5.4 Electronics Computer


interface
A variety of electronic subsystems are required to op-
erate an ion laser, as shown in the block diagram of Fig. 11.148 Block diagram of a large-frame ion-laser system
754 Part C Coherent and Incoherent Light Sources

Table 11.42 Ion-laser wavelengths


Powers available in a type of laser (W) (not all wavelengths are available simultaneously)
Available Lasing species Large-frame Mid-frame Large air-cooled Small air-cooled
wavelengths (nm) water cooled (W) water cooled (W) (W) (W)
275.4 Argon 0.375
300.3 Argon 0.5
Part C 11.5

302.4 Argon 0.5


305.5 Argon 0.17
333.6 Argon 0.4
334.5 Argon 0.8
335.8 Argon 0.8
350.7 Krypton 2.0 0.3
351.1 Argon 1.5 0.18
351.4 Argon 0.5 0.06
356.4 Krypton 0.5 0.12
363.8 Argon 2.0 0.25
406.7 Krypton 1.2 0.22
413.1 Krypton 2.5 0.3
415.4 Krypton 0.35
454.5 Argon 0.8 0.18 0.005 0.002
457.9 Argon 1.5 0.55 0.015 0.005
465.8 Argon 0.8 0.24 0.015 0.005
468.0 Krypton 0.5 0.1
472.7 Argon 1.3 0.32
476.2 Krypton 0.4 0.1
476.5 Argon 3.0 1.0 0.025 0.008
482.5 Krypton 0.4 0.05
488.0 Argon 8.0 2.5 0.1 0.03
496.5 Argon 3.0 1.0 0.03 0.012
501.7 Argon 1.8 0.64 0.015 0.005
514.5 Argon 10.0 3.2 0.1 0.025
528.7 Argon 1.8 0.55 0.01
530.9 Krypton 1.5 0.25
568.2 Krypton 0.6 0.25 0.02
631.2 Krypton 0.2
647.1 Krypton 3.0 0.8 0.015
676.4 Krypton 0.9 0.15
752.5 Krypton 1.2 0.15
793.1 Krypton 0.1
799.3 Krypton 0.2 0.03

that carry monitoring and control signals are typically almost 100 kg. These larger units may require cooling
bundled in the umbilical as well. water. Table 11.43 displays typical service requirements
Ion-laser power supplies show the same range of and loads for the three main classes of ion lasers.
variation in size and design as the laser heads. The power The electrical characteristics of the arc discharge
supplies of small air-cooled argon units can be as small are such that it essentially requires a constant-current
about 15 cm on a side, while supplies that drive large- supply in order to be sustained [11.1458]. The heart of
frame systems are roughly 0.7 m on a side and weigh an ion-laser power supply is the plasma current regulator.
Lasers and Coherent Light Sources 11.5 Ion Lasers 755

Table 11.43 Power supply characteristics of typical ion- flexible cable. Upon turn-on, all functions of the laser
laser systems can be accessed from the system controller. High-end
Ion- Max- Electrical Plasma Discharge
models offer a fully functioning computer interface for
laser imum input dis- power
automated remote operation and monitoring of the laser.
type laser charge require-
Ion lasers operate in either current mode or power
mode (also called light mode). Current mode holds the
power ment
plasma discharge current at a fixed value and allows the

Part C 11.5
Air- 20 mW 115 VAC 90 V 0.7 kW
laser output to vary. Power mode, a much more com-
cooled single phase 8A
mon method of operating the laser, adjusts the plasma
Small 5W 208 VAC 240 V 13 kW current as necessary to match the output power to a user-
frame three phase 55 A requested value. When the current can no longer be
Large 25 W 480 VAC 550 V 36 kW increased to achieve the power set-point, it may be time
frame three phase 65 A to replace the plasma tube.
Like many modern laser systems, most ion lasers
The plasma current needs to be well regulated in order are designed for hands-free operation. Air-cooled argon
to prevent line ripple and other variations from being systems in particular are intended to provide a con-
impressed on the laser output. The plasma current may stant laser source available from a simple flip of
be regulated by a linear transistor passbank, or more a switch. Large-frame systems in laboratory applica-
efficiently by various switching-type power supplies. tions in contrast trade on the flexibility they provide the
In the patented regulator used by Spectra-Physics, user.
a switched resistor regulator consisting of a pulse-width Small air-cooled systems continue to be economical
modulator (PWM) controlling a switch transistor is con- and reliable sources of coherent, polarized. TEM00 blue–
nected to a low-impedance high-power water-cooled green laser light. They are usually operated at a power
resistor. This resistor is connected to the plasma load. significantly derated from their maximum, which can
The PWM varies the percent of the time that the tran- extend their useful lifetime for years. Biological and
sistor is turned on and the resistor is conducting current. medical applications for these lasers include cell sorting.
A parallel capacitor provides a current path to the load Desoxyribonucleic acid (DNA) sequencing, bacterial
when the transistor is off. This regulator looks like analysis, confocal microscopy, and hematology. Many
a variable resistor that can vary from infinity down to of the dyes used in these applications were originally
the minimum resistance of the circuit. A shunt regula- developed for argon-laser wavelengths.
tor is used to provide ripple rejection and high-speed These lasers are also used in many applications re-
small-signal regulation. lated to producing text and images. The blue beam is
The power supply must power the electromagnet valuable for exposing printing plates for high-speed
when an axial magnetic field is employed. The electro- printing, and to provide the color separation required
magnet requires about 10–25% of the power supplied for full-color printing. Similar applications are found in
to the arc discharge. Thus a large-frame supply is really photoprocessing and other photographic sources.
two supplies: a 36 kW plasma supply and a regulated Mid-frame systems are used in many of the same
8 kW magnet supply. The power supply must also pro- applications as lower-power lasers. In addition, they are
vide power to heat the tungsten cathode in the plasma used in entertainment, especially for laser light shows,
tube. Typically a filament transformer provides 15–25 A and have laboratory applications in Raman spectroscopy
at about 4 VAC for this purpose. or as a pump sources for tunable laser systems such
as a Ti:sapphire. In ophthalmology, the beam can be
11.5.5 Ion-Laser Applications focused on the retina to repair diabetes – induced retinal
detachment, for instance.
The operator interface to control power and the basic The deep-blue and UV outputs of ion lasers have
on/off function is through the power supply. In inexpen- been used in the semiconductor industry for wafer in-
sive models of air-cooled systems, the control interface spection and lithography. The ability of the output to
typically consists of hand-wired knobs and switches on expose photoresist is also used in producing masters
the front panel of the supply. The next step in sophis- for compact discs, which then serve as the molds in
tication is a hand-held system controller with a visual the injection-molding manufacture of high-volume CD
display that attaches to the power supply with a long production.
756 Part C Coherent and Incoherent Light Sources

11.6 The HeNe Laser


The HeNe laser is an electrically pumped continuously nent. To achieve a beam quality comparable to the HeNe
emitting gas laser. Its basic principle is a gas discharge laser, however, requires considerable effort and addi-
in a glass tube filled with a mixture of helium and neon tional cost, which compensates for the higher costs of
under low pressure. The gas discharge is set up by a cath- a HeNe laser. For example, the strongly elliptical beam
ode and an anode placed at opposite sides of the glass of the diode has to be made circular and, in order to avoid
Part C 11.6

tube. The laser mirrors are usually fixed to the end of wavelength drift, temperature stabilization has to be pro-
the tubes. vided. Another advantage is the longer coherence length
The HeNe laser was one of the first lasers to be real- of a HeNe laser compared to that of standard diodes.
ized. It was developed in 1960 as the first laser emitting Further advantages of the HeNe laser are:
light continuously [11.1461]. However, this was not the
well-known bright red line (632.8 nm) that has been dis- • Excellent mode purity, typical > 95% Gaussian
covered, the first laser emitted light at 1.15 µm, which TEM00
is one of the strongest lines of the HeNe laser. Red laser • A favorable relation between resonator length and
emission was achieved shortly after, in 1962 [11.1462]. resonator width (diameter)
Though other possible transitions delivering light in the • A nearly diffraction-limited beam
visible had been found theoretically, it took a certain • High beam-pointing stability
time to demonstrate this practically. Improvements in • High reproducibility in manufacturing
resonator design and the performance of the mirrors
had to be achieved. Especially the well-known 543.3 nm 11.6.1 The Active Medium
line, with its low gain, needed several attempts by re-
searchers until it was demonstrated for the first time in Energy-Level Diagram
1970 [11.1463]. The most detailed energy-level diagram which we could
Shortly after its first demonstration, the HeNe laser find in the literature is given in [11.1465]. Nowadays,
found more and more applications and became the most however, the green and yellow laser lines are of much
common laser worldwide with millions of units sold, more importance than the infrared ones, so it was nec-
until laser diodes appeared on the market. More than essary to add these new visible lines to the diagram. It
40 years after its first appearance the HeNe laser is still of can be seen that neutral helium is excited by electron
great importance in the worldwide laser market. Around collisions and transfers its energy by nearly resonant in-
44 000 units were sold in 2005 [11.1464]. elastic atomic collisions to the excited states of neon.
The HeNe laser has been used for adjusting and This means that the lasing atom is the neon, helium is
positioning but also, because of its excellent optical only necessary for energy transfer from the gas discharge
properties, in interferometers, sensors or spectrometers. to the upper neon levels. The energy transfer from the
It was applied in the first scanner tills and even the first lower laser levels 3p and 2p ends at the 1s level due to
CD players were equipped with HeNe lasers. Although spontaneous emission and the 1s level is depopulated by
these applications have been taken over completely by wall collisions to the ground state of neon. For this rea-
diode lasers, HeNe lasers still find their use in many son it is necessary to have a small-diameter discharge
fields of analytics, instrumentation, sensor technology, tube, in order to secure a quick emptying of the 1s level.
science and education. It should be mentioned that the rare 3 He isotope is used
Its advantages are excellent beam quality, long and not 4 He. The reason is that the lighter 3 He isotope
lifetime and an unbeatable price–performance ratio. Be- has a higher velocity difference to neon, resulting in
cause of the mature technology and the still large sales better energy transfer to the upper laser levels [11.1466]
numbers manufacturing costs have decreased continu- and consequently a higher gain and output power (about
ously. Against the trend for shorter product lifetime the 25% better at 633 nm).
HeNe laser has asserted itself for 40 years and is still It is known that electron collisions and stimulated
a competitive product. Many OEM manufactures still absorption of visible light can cause transitions from the
choose the HeNe laser for there new products, irrespec- 1s to the 2p level, resulting in a higher lifetime of this
tive of the competition from diode lasers and solid-state lower laser level (2p). This leads to a higher inversion
lasers. Considering especially the laser diodes we see for the 3.39 µm laser line as for the other lines, since it
that, in fact, the diode itself is a rather cheap compo- has the 3p level as the lower laser level.
Lasers and Coherent Light Sources 11.6 The HeNe Laser 757

Table 11.44 Typical laser transitions


Energy (eV)
Wavelength Transition Gain Typical power
21 Helium Neon
(in air) (nm) (m−1 ) (mW)
1 2 3s 3.39 µm
543.3 3s2 –2p10 0.03 0.5–3.0 2 S0
5 3p
594.1 3s2 –2p8 2.0 1
Collisions 4
611.8 3s2 –2p6 0.1 2.0 2.4 µm 10
20

Part C 11.6
632.8 3s2 –2p4 0.5 0.5–50 2 3S 1 2 3s
0.5433 µm
640.2 3s2 –2p2 5
0.5941 µm
1.529 µm
1152.3 2s2 –2p4 2.0 E
1.15 µm 2p
l 1
1523.1 2s2 –2p1 4 1 e
19 0.6328 µm
3391.3 3s2 –3p4 100 10 c
t 4
r
o
n 10
Table 11.44 lists the commercially available laser
lines and some typical parameters. The gain [11.1465, 18 c
o
1467] depends strongly on the inversion and the noted l
values should only give an impression of how the gain l
i
changes with wavelength (g0 ∼ ν0−3 ). This illustrates s Possible excitation by
electron collision and
i
that the most difficult laser to build is the green one 17 o strong visible light
(543.3 nm). n
s 1s
2
Another difficulty in making a green laser is that,
5
within each group of energy levels (2s, 3s, 2p, 3p, and
so on), the energy distribution of the sublevels (e.g., 2p1 Wall
1 collisions
to 2p10 ) is determined by thermic Ne–Ne collisions, re- S0
0
sulting in a Boltzmann distribution, which means that
the population rises with falling energy. Thus, the lower Fig. 11.149 Energy-level diagram of the HeNe laser
laser level for the 543.3 nm line (2p10 ) has a much
higher population as the 2p4 level for the red line. In As shown in Fig. 11.149 the HeNe laser tube is filled
order to achieve population inversion for this laser line with a helium–neon gas mixture, having a total pressure
it is necessary to reduce the number of Ne–Ne colli- of about 4–7 mbar and a neon content of about 10%.
sions by reducing the neon pressure. The consequence The operating DC current is in the range of 3.5–11 mA
is a lower output power at this line and a lower lifetime and the corresponding tube voltage is about 1–5 kV.
for green lasers (about 10 000 h) compared to red lasers This is a cold-cathode glow discharge, where the active
(> 20 000 h). laser medium is formed by the positive column of the
Table 11.44 lists only the most important laser lines. discharge, which is located in a capillary of diameters of
A good compilation of laser lines at different elements is 0.5–2 mm. Since such a glow discharge has a decreasing
given in [11.213], which also contains references to the voltage–current characteristic curve (see Fig. 11.151),
original literature. Sometimes in an experiment one may
have unwanted light from scattering from the discharge
Laser tube
tube itself (not laser light). Such discharge lines can be
found in [11.1468].

Gas Discharge
R
The gas discharge is the most important process in the
laser, since it has to transform the electrical energy of
the power supply into the laser light. This process de-
termines the laser power, power stability, optical noise
and lifetime of the laser. Hence, the key know-how of U0
a laser manufacturer is not the resonator design but how
to optimize the discharge. Fig. 11.150 Electrical scheme of the laser
758 Part C Coherent and Incoherent Light Sources

trons depends on the properties of the cathode surface.


I
Normally the current density at the cathode surface is
constant, so the cathode surface must be large enough
for the applied operating current, otherwise sputtering
occurs and the tube is quickly damaged. The typical
cathode size is in the range of some 10 cm2 . In order
to avoid sputtering, at the surface a nanometer-scale
Part C 11.6

Working point layer of Al2 O3 is formed. Normally this oxide layer


withstands sputtering for some 10 000 h. If this layer is
destroyed, the laser fails within a few hundred hours.
IR
Ballast resistor 11.6.2 Construction and Design Principles

UT UI U0 U
Construction of a HeNe Laser
Figure 11.152 shows a cross-sectional view of a mod-
Fig. 11.151 Characteristic voltage–current curve of a HeNe ern HeNe laser. The principal setup is very similar for
laser all major manufactures of HeNe lasers and differs in
details only. The laser tube consists of a glass tube (8)
a ballast resistor R of about 60–100 kΩ is used to bring which is melted at both ends to metal end caps (3, 10).
the whole system to an increasing voltage–current curve. To these end caps the laser mirrors (1, 12) are connected
In Fig. 11.151 the black curve shows the electrical using a metal–glass soldering technique. These metal–
behavior of the discharge tube and the brown line the glass connections provide long-term vacuum sealing of
corresponding ballast resistor. After switching on the the laser tube. Inside the laser tube the cathode (6) and
laser, the power supply has to raise voltage to the ig- the gas discharge capillary (7) are located. The glass of
nition point (UI ≈ 10 kV). After the ignition, the power the capillary is melted to the glass of the outer tube (8),
supply switches to its normal fixed-current operating so the discharge is concentrated inside this capillary. If
mode. The corresponding voltage is determined by the the mirror (1) is a flat mirror and mirror (12) is concave,
crossing point of the discharge curve and the resistor the end of the capillary (9) acts as a mode field aperture.
line (voltage at the tube UT ). It is important to choose If linear polarized laser radiation is required, a Brewster
the resistor in such a way that only one crossing point window (2) is placed inside the laser. A favorable posi-
exists. tion for this window is near the flat mirror, because at
Whereas in the tube design a small metal anode is this position the beam diameter is the smallest in the tube
used, the cathode is considerably larger, and is mostly and there is no angular displacement between the laser
made of aluminium because the cathode has to deliver beam and the window (the beam is always perpendicular
the electrons for the discharge and to transfer the heat of to the mirror surface). The tube is evacuated and filled
the cathode fall, the region where the electrons are ac- using the pipe (4), which is sealed after filling the tube
celerated from zero to the colliding velocity, outside the by means of a cold soldering process. The spring (13)
laser tube. The capability of the cathode to emit elec- centers the capillary end. At the mirror holders (3, 10)

1 3 4 6 7 11 12

2 5 13 8 9 10

Fig. 11.152 Sectional view of a HeNe laser tube (LASOS Lasertechnik GmbH), see text for explanation
Lasers and Coherent Light Sources 11.6 The HeNe Laser 759

a region of reduced material thickness is formed (5, 11).


This is used for the alignment of the mirrors by means
of plastic deformation of the metal.
The setup according to Fig. 11.152 represents the
basic design of commercial laser tubes up to about
25 mW output power which has been used for about
three decades with minor changes only. It provides long-

Part C 11.6
term gas stability, clean optics over the whole lifetime
of the laser and a long lifetime of the laser.
In contrast to the present design, early HeNe lasers
were not sealed by the mirrors but by a Brewster win-
dow at each end. Thus, they used an external resonator,
mostly made of mirrors hold on invar rods. This older
design is used today only in high-power HeNe lasers
(> 35 mW), because such lasers need a very long cavity Fig. 11.153 Laser tube with fixed mirrors (LASOS Lasertechnik
(> 1 m). Here, the external resonator allows a better sta- GmbH)
bility of the mirror alignment, and the capillary (which
suffers from bending due to their own weight) can be The wave-front curvature at the output mirror is
aligned too. 2B
R= . (11.147)
D− A
Resonator Design
Using the well-known formalism for Gaussian beam
The design goal of a HeNe resonator is mainly to achieve
propagation, the beam diameter can be calculated at any
a Gaussian beam profile. The calculation of all beam
desired position.
parameters can be easily done by means of the ABCD
The complex parameter q is defined as:
matrix formalism [11.1469]. In this case, every optical
element in the laser is described by a matrix, as described 1 1 λ
= −i . (11.148)
below. q R πw2
The matrix of a mirror with curvature r
 
1 0
M= . (11.143)
−2/r 1

The matrix for the free-space propagation of dis-


tance s
 
1 s
S= . (11.144)
0 1

Starting at the output mirror all single matrices for every


element are multiplied for one complete round-trip (RT),
resulting in the following calculation:
 
A B
RT = S M2 S M1 = . (11.145)
C D

In a last step, the 1/ e2 beam radius (w) and the wavefront


curvature (R) are calculated from this matrix:
The beam radius at the output mirror is

λ 2|B|
w=  . (11.146) Fig. 11.154 35 mW laser tube with external resonator (LASOS
π 4 − (A + D)2
Lasertechnik GmbH)
760 Part C Coherent and Incoherent Light Sources

The propagation of a Gaussian beam through an mensions of the diode-lasers systems are much smaller
optical system described by the ABCD matrix yields (about 15 cm).
The product of the pressure p and capillary diameter
Aqin + B
qout = . (11.149) d is constant:
Cqin + D
pd = const. (11.151)
The beam diameter at the position of the mode field aper-
ture is important for the laser design (Fig. 11.155). The Following this equation, two systems with the same pd
Part C 11.6

ratio between this aperture and the beam diameter has product have comparable discharge properties and the
to be chosen in such a wa, that the losses for the TEM00 excitation of the upper laser levels is comparable in both
mode are low but high enough for the first higher-order cases if the same current is applied. This rule is very
transversal modes, e.g., TEM01 , in order to suppress useful if a well-running laser must be customized in
the higher modes. This ratio depends on the laser gain order to get more power or different beam diameter.
and can be calculated theoretically. The practical ex- If the new capillary diameter has been estimated using
perience for a common 633 nm laser leads to a ratio the formalism of Sect. 11.6.2 then the corresponding gas
between the aperture diameter and beam radius of about pressure for this new design can be calculated by means
3.5 : 1. For high-power HeNe lasers, this value must be of (11.151).
reduced, whereas for the low-gain 543 nm laser it has to The current–density scaling relation is less important
be increased. because there is only a weak dependence on capillary
In practical designs the above formalism is used to diameter
balance the resonator design between the beam diameter, √
4
required by the application (the beam waist is normally j d = const. (11.152)
located at the surface of the output mirror), and the laser
The scaling of the small signal gain g0 with capillary
power, which determines the laser length on one hand,
diameter d
and the available mirror curvatures as well the available
aperture diameters and aperture positions on the other. g0 d = const. (11.153)

Scaling Relations Equation (11.153) shows that a small capillary diameter


Scaling relations are very useful for the practical design d should be achieved in the design process because, with
of new lasers. The most important scaling relations are higher gain, losses can be higher too and it is possible
described below. Firstly, the laser power P, which is to come closer to the theoretical maximum power.
proportional to the discharge length l (capillary): Additionally two electrical relations [11.1470]
should be noted: the current density jK at the cathode
P
= const. (11.150) jK
l = const. (11.154)
p2
For this reason, today HeNe lasers with a power above
25 mW are very rare. These lasers are very long (> 1 m) and the ignition voltage UI
and need sensitive and expensive external resonators.  
pl
Thus, in this power region the costs for beam shaping of UI = f . (11.155)
T
laser diodes (aspheric lens systems with prisms, cylin-
drical lenses and/or zoom telescopes) are comparable Equation (11.154) has the consequence that low-
or lower than for a HeNe laser and the mechanical di- pressure laser tubes, like versions for 543 nm, need larger
cathodes. Equation (11.155) shows that the voltage nec-
essary to ignite the laser increases with pressure and
length and decreases with temperature T .

Laser Line Selection


Today, the HeNe laser has been replaced in the infrared
range by laser diodes, but its visible lines, especially
those at 632.8 nm, 594.1 nm and 543.3 nm, are widely
Fig. 11.155 Principle setup of a HeNe resonator with rear used in scientific applications such as laser scanning
and output mirror and a mode-field aperture microscopy. Because of this fact, we will only consider
Lasers and Coherent Light Sources 11.6 The HeNe Laser 761

the visible range. Except for some educational lasers,


Transmission (%)
all modern HeNe lasers operate at one wavelength only. 5
The reason is that it is only possible by this approach
to obtain the maximum power of each laser line and to 4
reduce the optical noise. The operating wavelength is
selected from the possible lasing lines by means of the 3
laser mirrors. In the most common design the rear mirror

Part C 11.6
has as high as possible a reflectivity (> 99.9%) for the 2
desired wavelength, and the output coupler will have
approx. 1–2% transmission at this line and > 10% at 1
the other lines. So, the unwanted laser lines have losses
greater than their gain and will not be amplified. Because 0
580 590 600 610 620 630 640 650 660 670 680
of the low gain of the 543.3 nm line, lasers for this Wavelength (nm)
wavelength must have output mirrors with transmissions
of about 0.05–0.15%. Fig. 11.156 Typical transmission curve of the output mirror
for a 632.8 nm laser
3.39 µm Suppression
From Table 11.44 it can be seen that the 3.39 µm line different processes. The first process is collision broad-
must be suppressed very carefully, because it has a gain ening, leading to a line width of about 500 MHz at typical
that is some orders of magnitude higher than all vis- pressures of 4–6 mbar [11.1466]. This line width is pro-
ible lines. Insufficient suppression of this line causes portional to the gas pressure. The second process is
power loss and power fluctuations at the desired lines. Doppler broadening (11.156)), which results in a width
Therefore, both laser mirrors must have a reflectivity for of 1–1.5 GHz for the visible laser lines.
this line below 0.5%. Another approach for the 3.39 µm A TEM00 laser usually runs at several longitudinal
suppression is to use the Zeeman effect. Applying an modes, which are spaced by
inhomogeneous transversal magnetic field to the laser c
splits the laser levels into the Zeeman sublevels. The ∆f = . (11.157)
gain of the sublevels is the gain of the unsplit level di- 2L
vided by the number of sublevels, so the gain may fall Thus, the longer the resonator (mirror distance L), the
below the losses and this line is suppressed. The fre- more modes can oscillate simultaneously.
quency difference of the sublevels is the same for all As can be seen in Fig. 11.157, the mode spac-
laser lines. However, Doppler broadening of the laser ing is 257 MHz (seven modes) and the gain profile is
lines depends on their frequencies. about 1.5 GHz. A Lamb dip does not occur because
The Doppler broadening of a laser line λ is given by the collision broadening is larger than the mode spac-
 ing [11.1466]. For interferometric purposes tubes that
2 2kT ln 2
∂νD = , (11.156)
λ m
where k is Boltzmann’s constant, T is the gas tempera-
ture and m is the mass of the Ne atom.
For visible wavelengths the frequency split caused
by the Zeeman effect is lower than the Doppler-
broadened line. Thus, the gain is not influenced by the
Zeeman effect, whereas for the 3.39 µm line the Zeeman
splitting is larger than the Doppler-broadened line and
the gain decreases with the number of sublevels. This
method is normally used in high-power 633 nm lasers
(> 35 mW) or in the 543 nm laser.
Fig. 11.157 Longitudinal modes (upper curve) and corre-
Line Width and Coherence Length sponding gain profile of a 584 mm-long 20 mW laser at
The natural line width of a red HeNe laser is about 633 nm (LASOS: LGK 7665 P), measured with a scanning
20 MHz [11.1466] but this line is broadened by two interferometer
762 Part C Coherent and Incoherent Light Sources

exhibit only one or two longitudinal modes are often Figure 11.158 shows the calculation of the meas-
used. The typical length of such a tube is about 140 mm ured contrast ratio of a longitudinal multimode laser
with a power of 0.5–1.0 mW. Whereas the gain curve is beam after a Michelson interferometer over the opti-
fixed in frequency space, the longitudinal mode pattern cal path difference. The beam was formed of four laser
shows a movement when the resonator length changes modes with equal intensity. This picture is overlayed by
in the dimensions of the wavelength λ, which may re- the decreasing contrast function of the single mode, but
sult from small ambient-temperature fluctuations. Such the coherence length of the single mode is in the range
Part C 11.6

a movement causes power fluctuations in the range of of kilometers and cannot be seen here. Whereas the in-
about 5% (depending on the laser length). Because in terference can be observed over very long distances, the
most applications only the sum power of all modes is periodic structure makes it necessary to define the coher-
used, it is possible to stabilize the laser power by in- ence length only in the region up to the first minimum.
creasing the number of modes under the gain profile. In the case of N longitudinal modes, this first minimum
This can be done by two methods. The first is to in- is located at the position
crease the laser length and the second uses a 1 : 1 mixture
2L
of the neon isotopes 20 Ne and 22 Ne instead of natural lmin = . (11.158)
Ne (90% 20 Ne and 10% 22 Ne). Because of the heavier N
nuclear core of the 22 Ne isotope the radiated light has Thus, for the laser of Fig. 11.157 the coherence length
a frequency about 800 MHz higher than the light from is below 16 cm.
20 Ne (isotopic shift, [11.1471] p. 333). This means that It should be mentioned that in a real laser the dif-
the difference between these two lines is smaller than ferent modes have different intensities, but this only
the Doppler broadening. Therefore, using a mixture of changes the amplitudes in Fig. 11.158 and leads to
these two isotopes gives a broader gain curve. The iso- a nonzero intensity at the minima.
topic mixture has no influence on other laser parameters
such as the power or noise. 11.6.3 Stabilization
One of the most exciting applications of the HeNe
laser is interferometry. For this purpose, the coherence In order to obtain a larger coherence length, a com-
length of the laser is important. The coherence length mon approach is it to use only one of the longitudinal
can by calculated from the line width ∆ν by modes. In order to select a single mode, the fact that in an
c unpolarized laser (without internal Brewster windows)
lc = . neighboring modes have perpendicular polarization di-
∆ν rections can be used. Hence, using a short unpolarized
The problem of a multimode laser is that it does not run laser with only two modes, it is possible to select one
at a single frequency but at several equidistant modes. mode by means of an external polarizer.
In some applications the frequency of this mode must
be fixed. This can be achieved by controlling the length
Kx
1 of the laser tube by means of a heater around the glass
tube. One way is to select the two perpendicular modes
0.8
using a polarizing beam splitter and measure the power

0.6

0.4

0.2

0
0 200 400 600 800 1000
x
Fig. 11.158 Contrast ratio for the interference of two four-
longitudinal-mode laser beams Fig. 11.159 Modes and gain profile of a 140 mm-long laser
Lasers and Coherent Light Sources 11.6 The HeNe Laser 763

Part C 11.6
Fig. 11.160 Components of a laser tube

difference between these two modes. By means of the process, where the processes of cleaning, connecting
heater, this signal should be held at zero. In this case and the vacuum processes are the key know-how of the
(Fig. 11.159) both modes are located at the sharp flanks manufactures.
of the gain profile. Here, small frequency changes re- After an initial cleaning process of the different
sult in large power changes and exact control of the components, in a first step the metal parts are soldered
frequency is possible. This principle is much easier than together in a high-temperature process (about 1000 ◦ C).
stabilizing a laser diode, at least with an external res- In the next step, the metal and glass parts are melted
onator with a grating, and the frequency depends only together at temperatures of about 800 ◦ C. During this
on the atomic properties of the neon. This first approach step, care must be taken that the capillary bore is at
to frequency stabilization is widely used in the field of the position of the subsequent optical axis. In order to
mechanical engineering for measurement devices with avoid mechanical stress, the different materials must be
an accuracy of about 1 nm. A detailed description of chosen in such a manner that the thermal expansion co-
frequency stabilization is given in Sect. 11.14. efficients of the metal and glass parts are matched. The
third step is soldering the mirrors to the mirror hold-
11.6.4 Manufacturing ers (at about 500 ◦ C). After this preparation, the tubes
are backed out under vacuum for many hours. Than,
Because the first HeNe lasers were built in the 1960s, by means of an oxygen discharge, the inner surfaces
today the manufacturing technology is a fully developed of the tube are cleaned of residual organic traces. The
764 Part C Coherent and Incoherent Light Sources

oxygen discharge is also used to form an Al2 O3 layer cells and allow the detection of abnormal structures. The
on the cathode surface, which is important for the life- working principle is that each particular fluorophore is
time of the tube. The next steps are filling the tube with excited by a special wavelength, emitting light at an-
the helium–neon gas mixture, carrying out a burn-in other wavelength, which is detected by highly sensitive
process and the final filling. In order to obtain laser sensors. Using various of these markers allows one to
emission, after these steps it is only necessary to align distinguish, label or sort cells. This method is applied in
the mirrors. A pre-alignment may be done by means basic research as well as in clinical diagnostics, where
Part C 11.7

of external lasers, using the back reflection of the laser it helps to detect serious diseases such as leukaemia or
mirrors from the tube, which should be adjusted. The acquired immune-deficiency syndrome (AIDS).
criteria for final alignment is maximization of the output Since most of these methods were developed in a pe-
power. riod when the only lasers sources available were gas
In order to get a robust product and/or because the lasers, the fluorescing substances were made especially
long high-power tubes are very sensitive to air flow, the for these wavelengths. Together with the common wave-
glass tube is usually connected to the ballast resistor and lengths of the Ar-ion laser they have become a kind of
both are placed in an outer aluminium tube. standard for this application, although a variety of other
wavelengths and corresponding dyes are also used to-
11.6.5 Applications day. The emission lines of the HeNe lasers are found
in nearly all commercial devices. Common applications
Most applications make use of the visible wavelengths of are flow cytometry and confocal microscopy.
the HeNe laser. Typical applications are flow cytometry,
confocal microscopy, DNA sequencing, sensing, haema- Interferometry
tology and photo-finishing. Last but not least the HeNe Interferometric methods are used for the precision mea-
laser is a very popular teaching apparatus in education, surement of various physical values. Examples are the
school or studies. A variety of applications use fluores- position or speed of particles, distances, stress or vi-
cence imaging and interferometry which are described bration. The optical properties and the long coherence
in more detail below. length of the HeNe laser make it ideally suited for
this kind of application. The narrow line width of the
Fluorescence Imaging laser allows its wavelength to be used as a measure-
Fluorescence imaging makes use of the different wave- ment standard. For many interferometric applications
lengths to excite fluorescence of certain fluorophores. the frequency of the emission line has to be stabi-
Particularly in biomedical applications this is one of the lized to achieve the maximum measurement precision
basic methods. Different fluorophores bind to specific (Sect. 11.6.3).

11.7 Ultraviolet Lasers: Excimers, Fluorine (F2 ), Nitrogen (N2 )


In 1984, Ch. K. Rhodes stated in the preface to the operation has therefore become possible, a prerequi-
world’s first book on excimer lasers [11.1472]: “The de- site for industrial applications. Together with laser-beam
velopment of excimer laser systems marked a significant monitoring and control by electronic means, the multi-
turning point in the development of coherent sources. disciplinary approach has made excimer lasers important
The progress of the last years has been largely predicated tools for a large variety of industrial and medical appli-
upon the combined knowledge of several disciplines cations.
including atomic and molecular physics, optical technol- For semantic reasons, the term excimer originally
ogy, and pulsed-power technology.” This early statement referred to excited dimers. Today it is used for all kind
was primarily associated with electron-beam excitation of laser-active media that are characterized by bound
of laser transitions of rare gases and rare-gas halogen excited states and dissociative ground states, more gen-
mixtures. Present excimer lasers are, however, based erally named exciplexes.
on precisely controlled electrical discharges, and rely This section is organized as follows. An overview
on detailed knowledge of material chemistry to assure of the unique properties of excimer lasers is followed
long service life of the discharge tubes. Cost-effective by a guide to the physics and technology behind these
Lasers and Coherent Light Sources 11.7 Ultraviolet Lasers: Excimers, Fluorine (F2 ), Nitrogen (N2 ) 765

laser systems, including beam characterization using


Energy (eV)
wavefront diagnostics. The section on applications fo- 12 10 8 7 6 5 4 3 2
cuses on the various techniques of material modification
Kr2
using excimer lasers and includes the use of fluorine Ar2 146 Xe2
(F2 ) laser radiation at 157 nm. The promising appli- 126 172
Rare gas
cations of femtosecond excimer laser pulses are also F2
157
considered. At the leading edge of current research, the Halogen KrCl XeBr [XeF(B–>X)]

Part C 11.7
chapter on ultrahigh-intensity applications deals with 222 262 351
ArF KrF XeCl XeF(C–>A)
the generation of hollow atoms and their application for 193 248 308 486±35 nm
Rare gas-halogen
ultrashort-wavelength X-ray generation. (diatomic) [Xe2Br]
Lastly, we present the new radiation sources at 440±30nm
Rare gas-halogen [Ar2Cl] [Ar2F] Kr2F Xe2Cl [Xe2F]
13.5 nm for next-generation lithography. Radiation (triatomic) 245±35 nm 285±25 nm 420±35 nm 490±40 nm 610±65 nm
sources in the extreme UV (EUV) can be realized by
both laser and discharge pumping and are expected to 100 200 300 400 500 600
Wavelength ë (nm)
transform the present microlithography into nanolithog-
raphy. Fig. 11.161 Wavelength (lower scale) and corresponding photon en-
Since the field of UV lasers is very large and has ergy (upper scale) of the various excimer transitions. The filled
recently been covered in a review book [11.1473] this symbols indicate commercially important wavelengths
short section just summarizes the various possibilities
and requests the reader to browse in [11.1472, 1473], bine via highly energetic transitions, thereby delivering
and in primary publications if more details are required. radiation in the extreme ultraviolet or weak-X-ray re-
gion. This is surely one of the most advanced promising
11.7.1 The Unique Properties applications.
of Excimer Laser Radiation Finally, excimer lasers are scalable to high pulse
energies in the joule range, to high repetition rates of
The most impressive property of excimer laser radia- a few kHz, to high average powers up to 1 kW, so that
tion is the large variety of emission wavelengths, which they can be conveniently adapted to specific industrial
cover the entire ultraviolet spectral region (Fig. 11.161). tasks. Compared to these facts, their drawbacks are the
The shorter the wavelength, the higher the resolution fairly broad line widths, the low degree of coherence and
that can be achieved in microprojection and -imaging, the non-continuity of the radiation. However, the latter
thereby opening a wide field of applications. Concur- characteristics are of minor importance considering the
rent with the short wavelength is the high quantum strengths discussed above. This leaves some space for
energy. Short-wavelength photons are strongly absorbed other lasers that might conquer the UV range by fre-
by most materials and they can supply sufficient quan- quency conversion, until more-powerful semiconductor
tum energy to induce photochemical reactions and cause emitters may partly fill the gap. The low degree of coher-
molecules to dissociate. Together with the high peak ence may be utilized for speckle-free imaging, and the
power available in a laser pulse, the bond-breaking broad line width, which enables ultrashort pulses, may
capability of excimer laser radiation allows ablative be narrowed by some frequency-selecting means in the
evaporation that opens the door to microprocessing of resonator setup. However, the beam, which somehow re-
many materials, ranging from soft biological tissue to sembles the emission of a lighthouse (large divergence),
hard diamond. requires some harnessing by beam-shaping optics.
The pulse duration is an important parameter. Typ- Figure 11.161 summarizes the data on wavelength
ical excimer lasers emit pulses in the range of a few and quantum energy of rare-gas halide lasers, together
nanoseconds so that material processing can be fre- with those of the fluorine laser and some other diatomic
quently performed on the fly, i. e., can be applied to and triatomic species. The F2 laser is actually not an
a continuous flow of components to be processed. In ad- excimer laser but can be excited in almost the same
dition, thanks to the naturally broad line width, excimer way. These UV sources are most important for a wide
lasers can be tailored to supply pulses in the femtosec- field of applications outlined in the next sections. The
ond range with extremely high peak power. This allows exotic types such as KrBr, rare-gas dimers and other
one to generate a plasma that consists of electrons and dimers as well as trimers are discussed in some detail
hollow atoms, i. e., inner-shell ionized atoms that recom- in [11.1472, 1473].
766 Part C Coherent and Incoherent Light Sources

11.7.2 Technology of Current Excimer Lasers the next shot so that rapid exchange of the laser gas is
and the N2 Laser required.
After the first experimental demonstration of
We start with the fundamentals of excimer lasers and a bound–free laser system in liquid Xe2 [11.1476],
the fluorine laser. Due to its role as a forefather of a large number of other excimer or exciplex molecules
all gaseous UV lasers, the (molecular) nitrogen laser were successfully investigated, including homonuclear
(N2 laser) will be briefly dealt with as well. Finally, the as well as heteronuclear species [11.1472], but most of
Part C 11.7

technology of discharge-pumped excimer lasers will be these did not gain importance for applications. The door
briefly outlined. to the systems listed in Fig. 11.161 was opened wide in
1975 [11.1477–1481], with convincing efficiency, wave-
Excimer Transitions: lengths, and after some technical effort, ease of handling
Unusual Four-Level Laser Systems of the laser gases. The gases are primarily the discharge
Excimer lasers derive their emission from molecules carrier, which is the buffer gas (mostly helium), and, to
that are generated a priori in an electronically excited a much lower extent, the reactants, which are the laser
state, which decays by emission of (laser) radiation into gases.
a repulsive or loosely bound ground state out of which
the molecule dissociates. In usual test-tube chemistry the Molecular Potentials and Reactions Kinetics
rare gases are noble or inert, i. e., they avoid chemical The rare-gas halide systems are characterized by two
binding, although special noble-gas compounds do exist electronic ground states, correlating with the electronic
also in the electronic ground state. The most important ground states of the rare gas and halogen atoms, which
molecules for commercially available excimer lasers are combine to a molecular Σ and a Π state, arising from
ArF∗ , KrF∗ , XeCl∗ , XeF∗ , where the asterisk refers to the p-hole of the halogen atom (Fig. 11.162 [11.1474]).
electronic excitation. Whereas the Π state is strongly repulsive, the Σ state
The dissociative electronic ground state is respon- shows a minimum, mostly with a depth of a few hundred
sible for the four-level character of these systems. cm−1 only, so that thermal energy allows the molecule
Generally, four-level laser systems can be operated in to dissociate within a few picoseconds. The first elec-
continuous manner. However, this is not possible with tronically excited states correlate with the positive rare
rare-gas halide excimer lasers because of physical and gas and negative halogen ions, and hence show a deep
technical restrictions. A fundamental one is the impor- minimum. The higher states correlate with the elec-
tant role that spontaneous emission plays with respect
to the stimulated emission in the ultraviolet spectral re-
Energy
gion; the ratio of the Einstein coefficient A, which is
responsible for spontaneous emission, and that respon- Structure of rare gas monohalides
sible for the stimulated emission in the same transition, M+ + X–
B, is proportional to the third power of the transition M* + X
frequency ν [11.1475]: Self M + X*
absorption
M+ X–(2Ó)-strongly bound,
A 2hν3 ionic like alkali halide
= 2 .
B c M+ X–(2Ð)
Broad
Hence stimulated emission can only compete with spon- band Laser transition (2Ó®2Ó)
taneous emission if the radiation intensity within the (2Ю2Ð)
transition I(ν) is so large that the product BI(ν) ex-
ceeds A, that is, if the system is pumped extremely M X(2Ð)-strongly repulsive, covalent
hard. Electrical power densities of some 100 MW/l must M+X
be deposited in the gas volume. In the early days, this M X(2Ó)-weakly attractive, covalent
excitation density was achieved by using energetic elec- thermally unstable
tron beams [11.1472]; nowadays short-pulse transverse
Internuclear distance
electrical discharges are being used. An extension of
the pulse duration beyond about 1 µs is hampered by Fig. 11.162 Typical potential energy diagram of a rare-gas
discharge instabilities caused by arcing. The detrimen- halide molecule. M stands for the rare gas, X for the halogen
tal reaction products and heat must be removed before atom [11.1474]
Lasers and Coherent Light Sources 11.7 Ultraviolet Lasers: Excimers, Fluorine (F2 ), Nitrogen (N2 ) 767

tronic excitations of the neutrals, and their potential is


shallower, as is typical for covalent binding. This gen- Discharge
Kr, F2
eral scheme holds for the rare-gas halides, except XeF
where the potential of the ground state reaches a depth
of 1065 cm−1 according to [11.1474].
In the buffer-gas-supported electrical discharge, the Kr, Kr*, Kr+
F2, F –
excited and ionic species are formed as shown for the

Part C 11.7
KrF∗ case in Fig. 11.163. The formation of the excited
Kr*, F2 Kr+, F –
rare-gas halide molecule follows both a neutral channel,
a chemical exchange reaction, and an ionic recombina-
tion channel, stabilized by third-body collisions with the (KrF)*
buffer-gas atoms. Hence the formation of exciplexes is Neutral branch Ion branch
favored at high pressure, i. e., pressures of a few bars.
The buffer gas also provides fast relaxation to the lowest Lasing 248 nm
vibrational level within the electronically excited state,
followed by a radiative transition to the ground state Kr, F
within a few nanoseconds.
The laser transitions couple with the continuum Fig. 11.163 Dominant reaction paths for the generation of
states above the ground state, showing a homogeneously KrF∗ [11.1482]
broadened non-Lorentzian line shape [11.1484]. Hence,
excimer lasers can be tuned within a certain bandwidth with a half-width of only 1.034 pm (FWHM, [11.1473,
range if frequency-selective optics are introduced – see Chap. 6, pp. 97]).
the tuning ranges in Fig. 11.161. The homogeneous line
broadening turns out to be favorable for the amplification Technical Design Principles for Excimer Lasers
of short pulses. From the physical preconditions described in the
In more detail, many more excited states that cor- two preceding sections it follows that the elec-
relate to the excited atomic states exist and are being trical energy of high density, on the order of
populated. However, their buffer-gas-induced relaxation 10−2 J/cm3 [11.1487], must be discharged homoge-
feeds the population of the lowest electronically excited neously into the laser gas (Fig. 11.165a) on a time scale
state. An overview of the reaction kinetics of both pure of a few nanoseconds so that a high-pressure (up to
rare gases and rare-gas atoms with halogens and the 0.5 MPa) glow discharge can be maintained for as long
underlying rate constants is given in [11.1474]. as possible.
The fluorine laser is based on bound–bound tran-
sitions. With 157 nm it shows the shortest wavelength
Intensity (arb. units)
of all homonuclear halogen lasers [11.1485]. From the 1
two p-holes of the F atoms, three levels belonging to 1
0.9 SNR=3828
ground electronic configuration are obtained for the 0.8
0.8 F2 spectrum
F2 molecule, two of which are bound, so that the sta- 0.6 FWHM=1.034pm
0.7 =12469.700MHz
ble molecule can be directly electronically excited in an 0.4 =0.4159cm-1
electrical discharge. In addition, excitation transfer from 0.6
0.2 E95%=2.867pm
the electronically excited He∗ and excited F∗ atoms, and 0.5 =34585.439MHz
=1.154cm-1
0
ionic recombination of F+ and F− ions, which have 0.4 157.628 157.630 157.632 157.634
Wavelength (nm)
a large electron affinity, during interaction with a He 0.3
atom lead to the population of the upper 3 Π laser level 0.2
that decays to the weakly bound lower 3 Π level. The 0.1
F2 laser transitions can be excited in discharges like 0
those in rare-gas halide lasers. Therefore the F2 laser 157.4 157.5 157.6 157.7 157.8 157.9 158
Wavelength (nm)
is frequently mentioned among the commercial excimer
lasers – in particular with respect to its short wave- Fig. 11.164 Emission spectrum of the fluorine laser accord-
length [11.1486]. Figure 11.164 shows details of the ing [11.1483]. Inset shows spectral details of the stronger transition
F2 laser emission together with a line-selected spectrum after line selection [11.1473]
768 Part C Coherent and Incoherent Light Sources

material research has taken place and led to different


a) Back materials for the fluorine and chlorine rare-gas lasers.
reflector
Output Even different materials for either the cathode or the
coupler anode, or over the profile of one electrode have been
used [11.1487]. Rapid transverse gas circulation pro-
vides cooling and supply of fresh laser gas for every
Discharge shot. In order to achieve stable laser output power,
electrodes
Part C 11.7

halogen gas consumption is compensated by processor-


Laser Glow
controlled gas injections so that the laser tube can be
beam discharge HV operated with a single main fill typically for about 1
pulser billion pulses.
b) Excimer laser resonators (Fig. 11.165a) mostly con-
sist simply of plane windows made of CaF2 , allowing
H.V. L 1S high out-coupling in the range 50–92%. For special
L0 C2 applications, unstable resonators or resonators with
Cp frequency-selective optics are employed, as well as
S
C1 oscillator-amplifier systems.
The number of technical papers on the technology
c) and construction of excimer lasers and their applica-
H.V. tions has become numerous. Excimer laser parameters
are scalable to a considerable extent. Special excimer
T L 0S L 1S L 2S lasers have been developed by putting in the fore-
PT
ground either high single-pulse energy (up to 10 J),
C0 C1 C2 Cp or high repetition rate (6 kHz), or medium or high
average power (up to 1 kW). The efficiencies, calcu-
lated from the ratio of laser output energy to stored
Fig. 11.165 (a) Schematic layout of an excimer laser electrical energy, are typically a few percent (< 5%).
together with gas discharge and laser resonator; (b,c) Ex- Since digital inter-publisher retrieval has become possi-
citation circuits employing magnetic pulse compression: ble [11.1490], nearly every combination of the above can
(b) L–C inversion circuit with single-stage pulse compres- be electronically traced back, in part, over the last three
sion, (c) thyristor-switched circuit using double-stage pulse decades. As an example, Table 11.46 shows data spec-
compression [11.1487] ified for an XeCl excimer laser designed for industrial
applications.
The electrical charge comes from a storage capacitor
or, more effective, a low-impedance pulse-forming line. Beam Characterization of Excimer Lasers
For a homogeneous ignition, an efficient pre-ionization For various applications such as the production of
is required. Pre-ionization by ultraviolet radiation has diffractive structures via direct patterning [11.1491,
prevailed over X-rays. Table 11.45 summarizes the dif- 1492], semiconductor microlithography or eye surgery,
ferent methods of UV pre-ionization. Glow discharges, a detailed knowledge of the wavefront of the emitted ex-
especially in halogen-containing gases, tend to trans- cimer laser radiation is necessary. In addition, all these
form into an arc or sparking discharge due to electron applications strongly rely on the stability and the precise
capture by the halogens so that laser emission breaks control of the laser parameters, such as pulse energy,
down. Hence, considerable efforts have been made to beam width, divergence, pointing stability, uniformity
stabilize the glow discharge [11.1488, 1489]. In order to etc. Thus reliable, standardized methods for the evalua-
supply the charge sufficiently fast, favorable use is made tion of beam parameters as well as accurate diagnostic
of magnetic pulse compression (Fig. 11.165b,c). The en- tools for UV laser beam characterization are mandatory.
ergy switches, formerly thyratrons, are mostly thyristors, While the output energy and the power can be moni-
gate-turn-off (GTO) thyristors or insulator gate bipolar tored with the standard tools that are used also for other
transistors (IGBT). high-power lasers, the recording of spatial beam pro-
To guarantee a long laser-tube lifetime, the choice files and directional distributions (wavefronts) requires
of electrode material is very important. Considerable specific instrumentation adapted to the characteristics of
Lasers and Coherent Light Sources 11.7 Ultraviolet Lasers: Excimers, Fluorine (F2 ), Nitrogen (N2 ) 769

Table 11.45 Pre-ionization techniques applied in excimer-laser discharges

Preionization of the laser gas by UV radiation emitted from spark discharges


between pin electrodes mounted in a row parallel to the laser channel. Sparks
are being ignited some 10 ns before the main discharge starts so that at least
108 electrons/cm3 are created as a seed for the main discharge.

Part C 11.7
A possible modification of a: spark preionization through one of the elec-
trodes designed as a screen or mesh electrode.

Dielectric(alumina)-surface-guided spark discharge for preionization. Be-


Ceramic
cause the discharge spreads, erosion of the pins is reduced considerably, thus
the lifetime of the laser gas is increased, and the laser tube can be operated
up to 10 billion shots. This design is mostly used in high-average-power
excimer lasers.

H.V. Surface corona discharges on a dielectric sheet emit UV with high spatial
uniformity. Consuming a lower amount of energy as compared to sparks,
they supply an electron density sufficient for a narrow discharge volume as
used in high-repetition-rate excimer lasers, and provide increased discharge
electrode lifetime.

H.V.

Knife-edge-released discharges creeping on a dielectric surface (similar to


the well-known Lichtenberg discharges) cover a large area, thus can be
conveniently applied for the preionization of large-aperture excimer lasers.
The knife edge is connected to the ground electrode of the main discharge.

H.V. Knife

Table 11.46 Data from an XeCl excimer laser for industrial use. (Type: Steel 2000, Coherent Lambda Physik 2005)
Maximum Maximum Maximum Pulse FWHM beam Divergence Beam point.
stabilized energy average power repetition rate duration dimensions V×H stability
(mJ) (W) (Hz) (ns) V × H (mm) (mrad) V × H (mrad)
1050 315 300 29 37 × 13 4.5 × 1.5 0.45 × 0.15

excimer lasers. Besides sensitivity to the various wave- stability of the employed optics and sensors under pulsed
lengths in the deep-UV spectral range, such diagnostic high-power UV irradiation. The evaluation of relevant
systems must also possess detector apertures adapted excimer beam propagation parameters is now possible
to the large near-field beam cross section of excimer with camera-based profile and wavefront measurements
lasers, and, most important, must guarantee long-term in accordance with current International Organization
770 Part C Coherent and Incoherent Light Sources

and shortly later between 300 and 400 nm with the


strongest line at 337 nm [11.1496] (described in detail
in 1965 [11.1497,1498]) quickly became the workhorse
for laser spectroscopy. Its predominant use was, and still
is, optical pumping of pulsed dye lasers throughout the
near-UV, the visible and near-infrared spectrum. In addi-
tion, it serves as an excitation source in photochemistry
Part C 11.7

and biological research. The lasing is achieved in high-


voltage (10–20 kV) high-speed (few-ns) transverse gas
discharges in a broad pressure range from some 10 mbar
up to atmospheric pressure (TEA laser), in pure nitro-
gen and also, with lower efficiency, in air. The 337 nm
transition is the most intense of the vibronic transitions
(0–0) between the C3 Πu and the B3 Πg states. Since
the B state is long-lived (about 10 µs) with respect to
the C state (about 10 ns), the laser action is quickly
self-terminating.
Fig. 11.166 Near-field (left) and far-field profile (right) The pumping is achieved from the X state by di-
of F2 laser (157 nm, Novaline F1030, Lambda Physik) rect electronic excitation of the C state, which happens
recorded simultaneously with a camera-based measurement to occur with a larger cross section than that for the
system. The evaluated second-moment beam widths in the B state, so that population inversion can be obtained
horizontal and vertical directions are also indicated if the discharge current rises much faster than radia-
tive increase of population of the B state. To emit pulse
for Standardization (ISO) standards [11.1493, 1494]. energies in the mJ range, N2 lasers must be equipped
Figures 11.166 and 11.167 show results obtained with with low-impedance discharge circuits, such as for ex-
a Hartmann camera-based measurement system. ample can be realized by embedding the laser channel
into a Blümlein transmission line, which enables a rise
Brief Recollection of the N2 UV laser time of a few nanoseconds. Since the gain is very large,
The molecular nitrogen laser, realized as early as the emission may be stimulated predominantly in one
1963 with emission in the near infrared [11.1495] direction when the excitation wave is made to reach
the discharge channel synchronous to the light propaga-
tion; in this way a 10:1 ratio in favor of one direction
can be achieved [11.1499], and fairly short lasers with
considerable peak output power (1.2 MW) are possi-
ble [11.1500]. Transmission line circuits are thoroughly
analyzed in [11.1501]. A pulse energy of 20 mJ has
been realized using a fast circuit with magnetic pulse
compression [11.1502]. On the other hand, just for
demonstration purpose, a nitrogen laser can be easily
203
realized by adjusting two electrodes on a glass sheet
W(ë) and supplying the electrodes with a spark-gap-switched
0
high-voltage source. A home-built nitrogen laser, using
28.8 standard ignition transformers, spark gaps, refrigerator
14.3
x(mm) circulating pumps, and some dielectrics and aluminium
y(mm) foil or copper-layered circuit boards, is precisely de-
0/0
scribed on the web [11.1503].
Fig. 11.167 Wavefront measurement of the emission of an F2 laser Historically speaking, N2 lasers as well as the
(157 nm) using a Hartmann camera (40 × 30 pinholes, diameter homonuclear excimer lasers and metastable mercury
100 µm, pitch 1 mm). This technique provides comprehensive beam compounds was proposed as early as 1960 by Houter-
characterization and propagation analysis of excimer lasers from mans [11.1504] – much earlier than the first ruby laser
a single measurement had been realized.
Lasers and Coherent Light Sources 11.7 Ultraviolet Lasers: Excimers, Fluorine (F2 ), Nitrogen (N2 ) 771

11.7.3 Applications line of thin-film transistor (TFT) displays. The prop-


erties 1–3 enable microstructuring by material ablation
Physically, the applications of excimer lasers can be including biological tissue, and property 4 opens the
grouped according to the benefits from door for the generation of X-rays of extreme brilliance.
Besides these technical applications, excimer laser radi-
1. short wavelength, and correspondingly, ation is still widely used for scientific purposes, such as
2. their high quantum energy, optical pumping of dye lasers. Here, we briefly refer to

Part C 11.7
3. the high pulse energy density obtained by focusing, a few of the technical applications.
and
4. the extreme peak power when the pulse energy is Excimer Lasers in the Electronics Industry
compressed into ultrashort pulses. Lithography for the generation of semiconductor circuits
has been based on excimer laser light sources for more
Property 1 allows exposing and patterning of sub- than a decade now, and will continue to do so for a couple
100 nm structures in photoresists for semiconductor of years. Thus this is the economically most important
lithography, property 2 allows photochemical near- application of these lasers. Because the diffraction-
surface modifications such as color change, as used limited minimum (half pitch) that is resolvable in optical
for marking of plastics, and index-of-refraction change projection is given by k1 λ/NA, every effort is made to
used for the generation of fibre Bragg gratings. Prop- decrease the wavelength λ for the illumination together
erty 3 allows the melting of thin silicon films, used with the process factor k1 , and to increase the numerical
to induce large-grain crystallization in the production aperture (NA) of the projection system. After extensive

2007 2010 2013 2016 2019


2005 2006 2008 2009 2011 2012 2014 2015 2017 2018 2020 2021
DRAM 1/2 pitch 65 nm 45 nm 32 nm 22 nm 16 nm

DRAM half-pitch
65 193 nm
193 nm immersion with water

Flash half-pitch

193 nm immersion with water


45 Narrow
193 nm immersion with other fluids options
EUV, ML2

EUV
32 193 nm immersion with other fluids and lens material Narrow
Innovative 193 nm immersion with water options
Imprint, ML2

EUV
22 Narrow
Innovative 193 nm immersion options
Imprint, ML2, innovative technology

16 Innovative technology Narrow


Iinnovative EUV, imprint, ML2 options

Research required Development underway Qualification/Pre-Production Continuous improvement

This legend indicates the time during which research, development, and qualification/pre-production should be taking place for the solution.

Fig. 11.168 Potential lithography exposure tool solutions according to the International Technology Roadmap for
Semiconductors 2005 [11.1505]. Courtesy ITRS
772 Part C Coherent and Incoherent Light Sources

dex of refraction higher than that of pure water are being


investigated. These could extend the use of 193 nm down
to a 30 nm half-pitch (see Fig. 11.169 from [11.1506]).
For the lasers to be used in lithography, there are
considerable requirements with respect to line width,
wavelength and pulse-to-pulse stability, lifetime of the
laser tube and all the optics [11.1508]. Dual-chamber
Part C 11.7

systems distribute the task of narrow-band generation


in the oscillator and power generation in the amplifier
tube; the latter can be designed as a regenerative ring
amplifier [11.1508]. Recently, a 60 W system operating
at 193 nm was introduced (Fig. 11.170 [11.1507]) with
the benefit of improved energy stability of the 6 kHz
pulses, so that the exposure dose of the resist can be
precisely controlled. This system aims for 45 nm half-
pitch production.
Transistors in thin films are the key elements to con-
Fig. 11.169 30 nm-wide lines and equally sized spaces ob- trol the individual pixels in displays. To increase the
tained at IBM Almaden Research Center (left) using 193 nm mobility of the electrons, large silicon crystal grains are
interferometric high-index immersion lithography, com- produced by applying excimer laser radiation to cause
pared to current 90 nm features. Courtesy IBM melting and controlled recrystallization, the beam be-
ing scanned in lines across the surface [11.1509, 1510].
use of 248 nm lasers, 193 nm illumination is now state of This process, summarized as excimer laser annealing
the art, and increasing the NA by using immersion op- (ELA), is performed by applying 308 nm radiation that
tics turned out to be a highly successful method to arrive is strongly absorbed by silicon so that thin films on glass
considerably below the diffraction limit. In the Interna- can be melted without damage to the substrate [11.1511].
tional Technology Roadmap for Semiconductors 2005 In this way, large-area TFT displays can be manufac-
(Fig. 11.168 [11.1505]) the 45 nm half-pitch for dynamic tured. Even doping imperfections due to incomplete
random-access memories (DRAMs) in production is annealing near source/drain junctions can be eliminated
scheduled for 2010, to be achieved with 193 nm im- by oblique-incidence ELA [11.1512].
mersion technology. Fluorine lasers (157 nm) are not in Further excimer laser applications that are well es-
discussion any more since immersion fluids with an in- tablished in electronics are printed circuit board (PCB)
via drilling [11.1513], wire stripping and wire mark-
ing [11.1473]. A rather new technology is the lift-off
Optical pulse
stretcher method to de-bond for example an electronic GaN LED
Linewidth analysis (OPuS)
module (LAM) MO from its sapphire substrate, which is used for crys-
WEB
tal growth, by shining the laser through the substrate,
MO chamber
thereby ejecting the LED onto its heat-sink electrical
interconnect [11.1514]. For future optical coupling of
Line narrowing
module (LNM) PCBs, attempts to integrate optical mirrors manufac-
tured by ablation should be mentioned [11.1515, 1516].
PA Auto
WEB shutter
PA chamber Processing of Optical, Ceramic, Polymeric,
and Biological Materials
Ablation is surely the best-known application of excimer
lasers: drilling and microstructuring of glass, quartz,
Bandwidth analysis even diamond, ceramics and polymers [11.1517] allows
module (BAM)
highly precise contouring with high reproducibility. This
Fig. 11.170 Schematic of a master oscillator power amplifier subject is covered in chapters 11–14 and 16 of [11.1473],
(MOPA) excimer laser system to be used in semiconductor lithog- which also includes the ophthalmological application in-
raphy [11.1507]. Courtesy Cymer Inc. cluding the laser-assisted in situ keratomileusis (LASIK)
Lasers and Coherent Light Sources 11.7 Ultraviolet Lasers: Excimers, Fluorine (F2 ), Nitrogen (N2 ) 773

method ([11.1473, Chap. 19], [11.1518]). Nonablative


processing of glass and polymers allows one to generate a)
Ti:Sapphire oscillator
fiber Bragg gratings in optical waveguides by changing
the index of refraction [11.1473,1519]. Microstructuring Ampli- Oscillator pump
is going to play a role also in the upcoming technology fier ù Frequency
pump stretcher tripling
of organic light emitting devices (OLEDs) [11.1520]. unit
Ti:Sapphire reg. amplifier
compressor

Part C 11.7
Femtosecond Excimer Laser Pulses 3ù
Another interesting subject of today’s excimer tech-
nology is their conversion into UV light sources with
femtosecond pulse duration. Basically a femtosecond KrF amplifier
seed pulse at 248 nm is injected into an appropriately
modified standard excimer laser resonator to achieve
a powerful highly directed short pulse emission. As 3 pass off-axis arrangement
examples are presented material processing with this
radiation and high-intensity studies for the generation
of tunable X-rays. b)
Conversion of a nanosecond excimer-laser system
into a fs system is described in [11.1521–1523] and
briefly in Fig. 11.171a. The ultrafast UV laser system
consists of a Ti:sapphire front laser, a frequency-tripling
unit to convert the wavelength of the ultrashort pulses
into the UV spectral range, and a specially designed KrF
amplifier to boost the energy of the pulses to several mJ.
The current laser arrangement, as shown in Fig. 11.171a,
uses a commercial Ti:sapphire front-end system (Coher-
ent) delivering pulses of 150 fs duration at a wavelength
of 745 nm. After frequency tripling, seed pulses are ob-
tained for the KrF amplifier module, which is the key
component of the system. This module is a modified
version of a commercial excimer laser. In a three-pass Fig. 11.171 (a) Layout of the UV femtosecond hybrid laser system
amplification scheme the pulses are amplified up to en- showing Ti:sapphire seed system and three-pass off-axis KrF am-
ergies of ≈ 30 mJ at repetition rates exceeding 300 Hz, plifier. (b) Comparison between calculated and measured surface
resulting in an average power of 10 W at 248 nm. textures for four-beam interference at a phase difference of 0π (left)
and 0.5π (right). The surface contours top left and bottom right were
UV femtosecond material processing. Nanoscale fab- measured via atomic force microscopy (AFM)
rication of materials is more and more in demand in
scientific and industrial applications. The general trend Such pulses are ideally suited for sub-micron ma-
to reduce the size of optomechanical devices and the chining of solid surfaces. Applying various diffractive
growing need for assemblies with feature sizes below optical masks in combination with reflective imag-
one micron generates new challenges for laser fabrica- ing/focusing systems allows the generation of complex
tion techniques. 2-D and 3-D structures with feature sizes down to
Short-pulse lasers with picosecond and femtosec- ≈ 200 nm or lower on all materials, including metals,
ond pulse duration offer material processing capabilities semiconductors and dielectrics. Figure 11.171 shows
with highly decreased damaged area around the irradi- the calculated and experimentally obtained surface
ated spot, and consequently smaller feature sizes. If the relief structures fabricated with the technique of phase-
short pulse duration is combined with short wavelengths, controlled multiple-beam interference [11.1524].
unprecedented results can be achieved due to the depen-
dence of the spatial resolution on the wavelength. Thus High-intensity UV femtosecond studies. A leading ap-
UV femtosecond laser systems provide superior material plication of KrF∗ (248 nm) excimer lasers has been the
processing quality. demonstration of saturated amplification in the multi-
774 Part C Coherent and Incoherent Light Sources

kilovolt X-ray regime that arises from the ability to was observed. These data confirmed that the selective
produce and controllably combine two new highly or- excitation of the inner-shell states initially observed
dered forms of excited matter: in N2 could be scaled into the multi-kilovolt spec-
tral region. A good example [11.1528, 1529] is given
1. hollow atoms and by the characteristic Xe(L) 3d2p hollow-atom emis-
2. stable electronically hollow plasma channels. sion profile centered at ≈ 2.8 Å shown in Fig. 11.172.
Hollow atoms are atoms (ions) that intrinsically pos-
Part C 11.7

The realization of this new X-ray source provides a peak sess an inverted electronic configuration consisting of
brightness that is sufficient for the implementation of deeply bound inner-shell vacancies, perhaps multiple,
a new high-resolution technology for biological mi- with the simultaneous retention of several electrons in
croimaging. relatively weakly bound outer orbitals. Accordingly,
these states are optimally suited for the prompt emis-
Hollow atoms and the cluster concept for X-ray am- sion and amplification of X-rays. The demonstration of
plification. Previous work [11.1526] on the nitrogen saturated amplification [11.1525, 1530–1532] followed,
molecule N2 suggested the possibility of designing a new together with the ability to form self-trapped plasma
class of molecular materials optimized for the efficient channels [11.1533, 1534]] that are well matched to the
production and amplification of X-rays [11.1527]. This conditions necessary for Xe(L) excitation in clusters.
idea was immediately tested with Xe clusters [11.1528]
with the outcome that the copious production of Xe Multi-kilovolt X-ray amplification with clusters in
hollow-atom states [11.1529] emitting both Xe(M) and self-trapped plasma channels. The fundamental
Xe(L) radiation in the kilovolt spectral region [11.1528] power compression and its spatial organization were
found in the alliance of the two basic phenomena men-
tioned above. They are
Intensity (arb. units)
160
Xe35+ 1. the direct multiphoton excitation of hollow atoms
Xe Xe34+
36+ from clusters with ultraviolet radiation and
140
Xe32+ 2. a nonlinear mode of stable confined propagation
in plasmas resulting from a relativistic/charge-
120 displacement mechanism of self-channeling [11.1533,
Xe31+
1534].
100 32+
Xe
The spectrum typical of the X-ray beam amplified
80 ds » 200 eV axially in the Xe plasma channel and recorded on
film with a von-Hámos-spectrograph is illustrated
60 in Fig. 11.173.
In Fig. 11.174 the axially recorded spectrum pre-
sented in Fig. 11.173 is compared to a transversely
40
observed single-pulse spectrum that exhibits deep and
broad spectral hole burning [11.1535] that corresponds
20
well with the axially amplified transition arrays. This re-
2.4 2.5 2.6 2.7 2.8 2.9 3.0 3.1 3.2 3.3 sult demonstrates two key attributes of the Xe(L) system,
Wavelength (Å)
namely,
Fig. 11.172 Characteristic spontaneous emission profile of
the Xe(L) 3d̃2p hollow-atom spectrum produced from Xe 1. a high efficiency of energy extraction and
clusters with intense (≈ 1019 W/cm2 ) femtosecond 248 nm 2. a very broad bandwidth (60 eV) for amplification.
excitation. The splitting between the major and minor lobes
arises from the spin–orbit interaction of the 2p vacancy. The In this case, the strongly enhanced lines observed cor-
full width of the main feature is ≈ 200 eV. The positions respond to the Xe34+ , Xe35+ , and Xe36+ charge state
of selected charge-state transition arrays (Xe31+ , Xe32+ , arrays of the major lobe shown in Fig. 11.172. These
Xe34+ , Xe35+ , and Xe36+ ) are indicated. The spectral observations, along with additional spectra showing
resolution of these film data is ≈ 4 eV. (After [11.1525]) comparable results on several other transition arrays in
Lasers and Coherent Light Sources 11.7 Ultraviolet Lasers: Excimers, Fluorine (F2 ), Nitrogen (N2 ) 775

Intensity (arb. units) Intensity (arb. units)


1.2 35+
1.2
Xe Xe35+
1.1 36+ Xe 34+ 1.1 36+ Xe34+
Xe Xe
1 1
0.9 0.9 Axial time-integrated
Xe(L) spectrum from
0.8 0.8

Part C 11.7
film #2
0.7 0.7
Transverse single-pulse
0.6 0.6 Xe(L) spectrum 030226B

0.5 0.5
0.4 0.4
0.3 0.3
0.2 0.2
0.1 0.1
0 0
2.4 2.5 2.6 2.7 2.8 2.9 3.0 3.1 3.2 3.3 2.4 2.5 2.6 2.7 2.8 2.9 3.0 3.1 3.2 3.3
Wavelength (Å) Wavelength (Å)
Fig. 11.173 Axially recorded spectrum showing sharp peaks Fig. 11.174 Comparison of the axially detected film #2
at the positions of the Xe34+ , Xe35+ , and Xe36+ transition shown in Fig. 11.173 with a single pulse spectrum
arrays. On the basis of geometric considerations concern- (#030226B) recorded transversely, illustrating deep spec-
ing the von-Hámos-spectrograph and the ratio of exposures tral hole-burning corresponding to the region of the Xe34+ ,
corresponding to the spontaneous signal and the amplified Xe35+ , and Xe36+ arrays. Since the hole burning descends
lines, the recorded enhancement of these features is esti- to the noise level of the detector, efficient energy extraction
mated to be minimally ≈ 1.5–3.0 × 103 over the strength is evident. The width of the spectral gap is ≈ 60 eV, a value
of the spontaneous emission sufficient for amplification of a pulse with a duration of
≈ 30 as
the ≈ 2.71–2.93 Å region, indicate that the hollow-atom
states are strongly inverted and that the amplification which are the ultraviolet and X-ray waves propagating
can be tuned across a substantial fraction of the spec- in the channel. The chief consequence is well-ordered
tral profile illustrated in Fig. 11.172. An estimate of the and efficient energy flow conducted through radiation-
peak spectral brightness achieved in the initial experi- dominated interactions that are confined to a small
ments [11.1525] gave a value of ≈ 1031 –1032 photons phase-space volume. Finally, it is significant to note
(s mm 2 mr 2 )−1 and (0.1% bandwidth)−1 , a range ap- that ordered energy flow was the principal character-
proaching that required for single-molecule imaging in istic of excimer systems that made [11.1472] them so
living biological material [11.1536–1538]. abundantly useful over the last three decades. Hence,
In summary, the study of high-intensity interactions a key feature of that history appears prominently again
with ultraviolet excimer lasers on atoms, molecules, in the X-ray range.
and plasmas over the last 20 years has culminated
in the ability to produce new forms of matter that 11.7.4 Outlook:
are both highly excited and highly ordered [11.1539]. Radiation in the EUV
A consequence is the capacity to achieve saturated
X-ray amplification in the multi-kilovolt regime at peak The roadmap of the semiconductor industry (Fig. 11.168)
brightness figures sufficient for the implementation of shows in which way computer chips with critical
biological microimaging. Basically, the amplification dimensions of 32 nm and below are planned to be
proceeds through the creation of a highly ordered ex- manufactured: light sources with emission in the ex-
cited state [11.1525, 1535] that is comprised of four treme ultraviolet (EUV) at a wavelength of 13.5 nm will
mutually coupled components: atomic (ionic) matter, be used. EUV lithography is considered as the next-
plasma electrons, and the two coherent radiative fields, generation lithography (NGL) to be established after
776 Part C Coherent and Incoherent Light Sources
Part C 11.7

Fig. 11.175 EUV microexposure tool from Exitech with an


integrated EUV source from XTREME technologies (left)

reaching the physical limits of ultraviolet (immersion)


lithography based on ArF excimer lasers.

13.5 nm Technology
The first EUV microexposure tools are already under Fig. 11.176 EUV plasma source integrated into an optical
operation for technology development and feasibility system
studies (Fig. 11.175).
One of the biggest challenges concerning the in- mogeneously emitted radiation from such plasmas is
troduction of EUV lithography is the development of pulsed with lengths in the nanosecond range (typically).
high-power EUV sources at a reasonable cost. Mak- The distribution of the wavelength spectrum is narrow
ing the operation of the photolithography manufacturing from elements with low atomic numbers and broad from
tools economically viable requires a source with power elements with high atomic numbers. In addition, the ra-
in the kilowatt range at the 13.5 nm exposure wave- diation is almost fully incoherent, as from a thermal
length. In addition, the optical design of the collector Planck emitter.
optics sets limits on the source size, i. e., an emission Today the highest EUV power is achieved in so-
volume of a few cubic millimeters. Only the combina- called pinch plasma sources. However, the heat load on
tion of both the high power and small emission volume the static electrode configuration can lead to fast erosion
will enable high optical efficiency and therefore high and even melting of the surfaces, thereby limiting the
wafer throughput. The goal is the development and power scaling through increasing repetition rates. Alter-
manufacturing of these high-power EUV sources as native technologies with moving electrodes have been
well as their integration into the optical system of the investigated and finally a potential solution with rotating
photolithography tool (Fig. 11.176). disc electrodes (RDE) has been found. A new excitation
Plasmas are known as efficient emitters of 13.5 nm scheme has been applied to this technology at XTREME
EUV radiation, if their temperature reaches about technologies, resulting in a world record (170 mJ/2π sr)
200 000 ◦ C, i. e., approximately 35 times higher than of the achieved EUV pulse energy [11.1542]. This effect
at the surface of the sun. Plasmas can be generated ei- resulted in a reasonable repetition rate to fulfill the power
ther by an electrical discharge or by means of pulsed requirements of high volume manufacturing tools. Fur-
laser excitation. Both methods are able to generate small ther development efforts will be directed to combine the
plasma volumes fulfilling the technical requirements power-scaling capability with the reliability goals for
of photolithography [11.1540, 1541]. The spatially ho- this concept.
Lasers and Coherent Light Sources 11.8 Dye Lasers 777

11.8 Dye Lasers


11.8.1 Overview tially, continuous tunable laser action can be obtained
from the near ultraviolet to the near infrared. Typi-
The distinctive feature of dyes as a lasing media is the cally a strongly absorbing and strongly emitting dye
broad emission band with a typical bandwidth of 50 nm. is dissolved in a suitable solvent (e.g., a polar solvent
Laser action from dye molecules was first observed by such as ethanol or a nonpolar solvent such as chloro-

Part C 11.8
several research groups in 1966 [11.1543, 1544]. Com- form) at concentrations of 10−3 –10−4 molar to serve as
pared to the gas and solid-state lasers of the 1960s, the gain medium. A flashlamp or another laser is used
dye lasers easily excelled both in terms of broad spec- as the pump. Powerful coaxial flashlamp-pumped rho-
tral coverage and in versatility of output performance damine 6 G dye lasers can deliver laser energy up to
(viz. high per-pulse energy output, long or short pulse 400 J per pulse [11.1546]. Average output power of up
operation, flashlamp or laser pumping) Researchers to 1.2 kW in burst mode were obtained in a flashlamp-
quickly recognized the wavelength tuning capability of pumped dye laser by Morton and Dragoo [11.1547].
dye lasers, which is probably one of the most impor- Since the advent of high-power short-wavelength lasers
tant operation characteristics in view of applications. In in the 1970s, excimer, nitrogen or frequency-multiplied
the following years, literally hundreds of organic dyes Nd:YAG lasers are frequently used for pumping liquid
with emission spectra from the near ultraviolet to the dye lasers with output pulse around 10 ns and energy
near infrared (300–1200 nm) have been made to lase. output of tens of millijoules. A saturable absorber (an-
Continuous-wave (CW) or ultrashort pulse (femtosec- other dye) is used to passively mode-lock the dye laser
onds) operation of dye laser was also demonstrated. With to generate pulses of about 200 fs without dispersive
their broad spectral coverage and narrow linewidth tun- elements and down to tens of fs with dispersive op-
ability, dye lasers have been the workhorse in scientific tical elements [11.1548]. For applications that require
laboratories for applications ranging from fundamen- single-longitudinal-mode laser output, CW operation of
tal physics to clinical medicine for many years. Despite dye lasers is achieved by using a modified flow system
the bad reputation of being prone to various mishaps to remove the long-lived triplet state of the dye mol-
during operation (e.g., spilling of dye solution being ecule. The linewidth of a free-running jet-stream CW
a not infrequent occurrence), there are many loyal fans dye laser can be as low as to 2 MHz [11.1549]. In the
of liquid dye lasers in the scientific community. This following sections, we discuss several common dye laser
popular support is a tribute to the versatile output per- arrangements.
formance of these liquid lasers and the simplicity of
the technology involved in constructing a liquid dye 11.8.3 Flashlamp-Pumped Dye Lasers
laser. Almost any research lab can put together a flash-
lamp with power supply, two mirrors, some common A flashlamp was the pump source for Maiman’s epoch-
dye (e.g., rhodamine 6 G), and nuts and bolts to build making ruby laser. Today’s flashlamps are still used
a pulsed liquid dye laser. There are of course numerous to pump liquid and solid-state lasers. Linear flash-
user-friendly and powerful liquid dye lasers available.
We will first give a short description of the charac-
Total reflector
teristics of liquid dye lasers and then discuss several
types that are commonly found in research laborato-
ries for photophysical, photochemical and spectroscopy
applications. Reflectors

11.8.2 General Description


Laser
Dyes are organic compounds that contain conjugate dou- output
Coaxial
ble bonds. The presence of the conjugate double bonds flashlamp
renders these compounds optically active. There are over Dye cell
Output coupler
200 laser dyes that can, in principle, provide spectral
coverage from 320 to 1200 nm [11.1545]. The tuning Fig. 11.177 Schematics of a coaxial flashlamp-pumped dye
range of each dye is 40–60 nm. When used sequen- laser
778 Part C Coherent and Incoherent Light Sources

lamps are often the choice for laser pumping and 11.8.4 Tunable Dye Lasers Pumped
usually consist of a tubular quartz envelope sealed by by High-Power Short-Wavelength
tungsten electrodes at both ends. The tube is often Lasers
filled with a heavy rare gas (e.g., xenon or kryp-
ton) for high electrical-to-optical conversion efficiency. By incorporating wavelength-selective elements inside
Still close to 90% of the electrical power ends up the resonator cavity, dye laser output can be tuned.
as heat, which requires a cooling system for its re- Increasingly excimer or frequency-multiplied Nd:YAG
Part C 11.8

moval. Often, an elliptical reflector is used to focus the lasers are used to pump dye lasers. Excimer, nitrogen
output from the flashlamp into the dye cell. For op- and frequency-multiplied Nd:YAG lasers all provide
timum coupling of the light from the flashlamp into high pump power (peak power of several MW) at
the dye, the dye cell must be placed close to the lamp. short wavelengths, making them highly suitable for
Coaxial lamps have emitting surfaces that completely pumping dye lasers. Dye lasers pumped by high-power
surround the flowing dye. Figure 11.177 shows a coax- short-wavelength lasers exhibit such high gain that loss
ial flashlamp-pumped dye laser, a structure commonly introduced by the additional wavelength-selective el-
employed in many commercial dye as well as solid- ements inside the resonator cavity can be overcome.
state lasers. The dye cell is set at the center of the Either prisms or diffraction gratings can be used for
coaxial, cylindrically shaped xenon flashlamp for op- wavelength selection, and gratings are generally superior
timal pumping. Two broadband mirrors provide the in terms of large dispersion and wavelength-resolving
optical feedback. Such a flashlamp-pumped dye laser power. Figure 11.178 shows a variant of the telescopic
typically produces a broadband emission (about 10 nm grating resonator originally used by Hänsch [11.1550]
linewidth) centered at the peak of the gain profile for the generation of narrow-linewidth laser output.
with a pulse duration of 1–2 µs. The output energy is A nitrogen laser provided the pumping. The use of the
about 100 mJ for most commercial flashlamp-pump dye telescopic lens increases the number of grooves illumi-
lasers. nated by the laser light and reduces the light intensity
on the grating, preventing damage to the coating on the
grating surface. The linewidth of a telescopic-grating
Dye cell cavity dye laser is in the range of 0.1 nm. To further
Telescope
Polarizer Laser reduce the linewidth to 0.01–0.05 nm, an intracavity
output
etalon (e.g., a coated optical flat or air-spaced Fabry–
L1 Pérot cavity) may be introduced. Many variants of the
Grating M1
L2 grating-cavity (e.g., the hybrid prism–grating cavity) dye
Pump
lasers have been developed to achieve narrow-linewidth
Fig. 11.178 Schematics of a Hänsch-type cavity dye laser. A tele- output [11.1551].
scopic lens is used to improve the spectral resolving power of the
grating 11.8.5 Colliding-Pulse Mode-Locked Dye
Lasers

Laser dye jet The broad emission band of a dye can be used ef-
fectively to generate ultrashort laser pulses, since the
Dispersive
prism theoretical limit of the ultrashort-pulse duration sup-
ported by the gain medium is proportional to the inverse
Pump of the gain bandwidth. As the emission bandwidth of
many laser dyes is 40–50 nm, pulse durations down to
tens of fs can be produced. The development of passive
Flat output mode-locking is essential to the successful demonstra-
mirror
Astigmatically tion of femtosecond pulse generation in dye lasers. In
compensated passive mode-locking, a saturable (nonlinear) absorber
cavities Saturable
absorber dye jet (an absorbing dye) with an absorption that matches the
emission wavelength of the lasing dye is placed inside
Fig. 11.179 Schematic of a colliding-pulse dye laser for ultrashort- the resonator cavity. Ideally, the leading and trailing
pulse generation edges of the optical pulse are removed by the absorber
Lasers and Coherent Light Sources 11.8 Dye Lasers 779

whilst the peak of the pulse, unaffected by the absorber,


Thin Thick Birefringent
experiences amplification. The efficiency of the absorber etalon etalon filter
increases considerably if two oppositely traveling pulses M3
interact or collide in the saturable absorber at the same M2
time (colliding-pulse mode locking). This is a result of
Laser
the two coherent pulses interfering constructively, lead- output
ing to the reduction of power required for the saturation Laser dye jet Brewster
tuning plate

Part C 11.8
of the absorber. The colliding-pulse mode-locking con-
figuration can be realized in either a linear or ring cavity.
M1
Because of the ease of alignment, the ring cavity is Mp
Pump
often preferred. Figure 11.179 shows the type of ring
laser used originally by Fork et al. to generate pulses Fig. 11.180 Schematic of a linear-cavity CW dye laser for single-
shorter than 100 fs [11.1552]. Both the laser dye (e.g., mode operation
rhodamine 6 G) and the absorbing dye (e.g., DODCI)
are in the form of a free-flowing stream jet, and a CW
argon-ion laser serves as the pump. The radii of curva-
Laser dye jet
ture of the mirrors must be carefully chosen so that the Pump

spot size in the absorber is smaller than that in the gain


medium to assure pulse-forming stability. Double Brewster
tuning plates
11.8.6 Tunable Continuous-Wave Dye Lasers

The linewidth of tunable pulsed dye lasers with intracav-


ity dispersive element for narrow-linewidth operation
are of the order of 500 MHz. In contrast, a continuous- B
wave dye laser is capable of delivering laser output with Laser
linewidths as narrow as tens of kHz. The high resolving output
Optical diode Thin Thick Birefringent
power is ideal for spectroscopy. Such high performance (Faraday isolator) etalon etalon filter
is connected with high cost, complicated design and
a high-power pump source (often a CW argon-ion laser Fig. 11.181 Schematic of a ring-cavity CW dye laser for single-mode
with 10–20 W output power). Continuous-wave dye operation. Note the use of an optical diode to assure unidirectional
lasers have much lower gain than their pulsed counter propagation of the traveling wave
part. The loss reduction becomes critical and the re-
moval of the long-lived triplet state is crucial for the narrow-linewidth output. The birefringent filters are for
stable operation of the laser. A free-flowing jet is used wavelength tuning. A ring-cavity supports the propaga-
to effect rapid circulation of the dye. Since the gain pro- tion of traveling waves and thus is ideal for single-mode
file of most dyes may be regarded as homogeneously operation. Figure 11.181 shows a tunable single-mode
broadened, one might expect single longitudinal-mode ring laser supporting single-mode operation. The op-
output from a simple grating or prism-cavity CW dye tical diode (a Faraday isolator) ensures unidirectional
laser. However, single longitudinal-mode operation may travelling waves thus avoiding spatial hole burning.
not be possible in such linear-cavity dye lasers with-
out intracavity frequency-selecting elements because 11.8.7 Advanced Solid-State Dye Lasers
spatial hole burning can arise gain saturation by the
standing wave. Multimode output then results. Addi- The contribution of liquid dye lasers to the advance of
tional frequency-selecting elements such as an etalon laser technology, particularly to ultrafast laser technol-
must be inserted inside the cavity for single-mode op- ogy and the many applications of tunable lasers, cannot
eration increasing losses and lowering output power. be overstated. Interested readers should consult mono-
Figure 11.180 shows a linear (standing-wave) cavity graphs such as Dye Lasers by Schäfer [11.1553] or Dye
arrangement for a CW dye laser end-pumped by an Laser Principles by Duarte and Hillman [11.1554] and
argon-ion laser for single-mode operation. The dye jet references therein for more detailed information on the
flows perpendicularly to the page. The etalons assure range of applications of dye lasers. The excellent out-
780 Part C Coherent and Incoherent Light Sources

put performance (as mentioned in the last paragraph) were shown to have good chemical stability and wide
notwithstanding, dye lasers earn skepticism among their optical transparency for use as host materials for laser
users. The main misgivings for dye lasers in liquid form, dyes. The pace of research activity has increased con-
may be the disposal of the used dye and the maintenance siderably since then. In the sections to follow, we will
problems associated with the physically large circulation bring the reader up to date with the latest development of
loop for the dye flow. With the emergence of transition- solid-state dye lasers. The state of the art of solid-state
metal solid-state lasers in 1980s, the position of dye dye lasers based on pure and hybrid sol-gel materials and
Part C 11.8

lasers as the tunable laser-light source of choice has been on advanced polymers is covered in the next section. The
facing a rising challenge. These solid-state lasers are most current development of solid-state dye lasers may
based on the vibronic transitions of 3d transition-metal be polymeric [11.1561] or sol-gel [11.1562] waveguide
ions such as Cr3+ , Ti3+ , and Co2+ doped into oxide lasers using a distributed feedback configuration. These
or fluoride crystals that served as the host [11.1555]. compact lasers produce tunable narrow-linewidth output
These transitional-metal ion-doped crystals show broad and appear to be readily integrable into planar optical
emission bands (typically 200–300 nm) in the visible to circuits. This is covered in the penultimate section. Fi-
near-infrared spectral region and thus are good tunable- nally the topic of tunable upconverted DFB dye lasers is
laser candidates. The most well known among them is presented.
the Ti3+ :Al2 O3 (titanium:sapphire) laser. Tunable ra-
diation in the blue–green and in the ultraviolet can in Solid-State Dye Lasers Based on a Polymer Host
principle be obtained by frequency doubling or tripling In 1967, one year after the demonstration of the
the fundamental output of Ti3+ :Al2 O3 lasers. In addition first liquid dye lasers, Soffer and McFarland observed
optical parametric oscillators (OPO) based on nonlin- lasing in rhodamine-doped poly(methyl methacrylate)
ear optical crystals such as ADP or BBO (BaB2 O4 ) (PMMA) [11.1563]. The first polymeric hosts suffered
are capable of providing tunable radiation well into from large thermal coefficients, stress birefringence, op-
the infrared [11.1556]. The leading role of dye lasers tical inhomogeneity and chemical reactivity with laser
as a tunable coherent-light source is indeed somewhat dyes. The most serious problem of dye-doped poly-
diminished. mers is the tendency of aggregation of dye molecules,
which effectively quenches fluorescence. As a result,
Challenges and Opportunities the performance of the initial solid-state dye lasers
Solid-state lasers are often preferred because of their was less than satisfactory. The properties of PMMA
ruggedness and easy maintenance. User-friendly dye can, however, be improved by purification of the
lasers must do without the flow loop that circulates the monomer, by introducing alcohol additives [11.1560]
dye solvent. Solid-state dye lasers (SSDL) incorporating
the dye molecules in solid matrices appear to be able to
Holographic grating
combine the cost-effectiveness of liquid dye lasers and
Aperture
the ruggedness of inorganic solid-state lasers. In order Lens
for SSDL to be a serious competitor to inorganic solid- Laser pump
state lasers in various fields of applications, the problem
of photodegradation of dye molecules must first be dealt Mirror
with.
Good progress has been made in the synthesis of Dye-doped
sol-gel film Mirror Mirror
photostable dyes. The recently synthesized perylene
family [11.1557] and the pyrromethene family [11.1558]
of laser dyes have been shown to outperform rhodamine-
6G in efficiency, tunability and photostability. Equally è
important to the development of SSDL are the solid-
Glass substrate
state matrices that serve as host materials where there
has also been impressive progress. In the 1980s Avnir DFB output DFB output
et al. [11.1559] and Gromov et al. [11.1560] demon- Dye-doped sol-gel waveguide
strated dye-doped sol-gel materials and dye-doped
polymeric materials, respectively, as promising laser Fig. 11.182 Experimental arrangement of a sol-gel DFB
media. Both sol-gel materials and polymeric materials waveguide dye laser
Lasers and Coherent Light Sources 11.8 Dye Lasers 781

and can be modified through copolymerization with ganic precursors is mechanically fragile and optically
a low molecular-weight polymer [11.1564]. The result is lossy due to the presence of numerous pores. The use
an improved polymer: modified poly(methyl methacry- of organically modified precursors or organic modifiers
late) (MPMMA) with the desired optical homogeneity during the sol-gel process results in organically modified
and chemical stability suitable for use as a solid-state silicates (ORMOSILs) that show improved mechanical
dye laser host [11.1565]. Work on the development strength and much reduced optical loss [11.1565,1566].
of new polymeric hosts has been very active. King The combined use of the improved sol-gel materials as

Part C 11.8
and coworkers showed that the photostability of solid- host and the deoxygenation procedures during sample
state dye lasers can be enhanced by deoxygenation of preparation has lead to sol-gel dye lasers with lifetime
the host [11.1566] and the addition of a triplet-state exceeding one million shots [11.1573].
quencher [11.1567]. Following the idea that photodegra- One of the attractions of sol-gel materials is the
dation of dye molecules can be reduced by increasing the potential that such glassy materials can have prop-
rigidity and hence the rate of heat dissipation of the host erties similar to glasses made via the traditional
matrix, Costela et al. [11.1568] prepared pyrromethene high-temperature approach. Another attraction is the
dye-doped copolymers of methyl methacrylate (MMA) ability of sol-gel materials to trap both organic and
and different methacrylic and acrylic crosslinking poly- inorganic dopants while showing exceptional chem-
mers. The combined use of a photostable dye and new ical stability. Whilst very few polymeric dye lasers
polymeric hosts results in SSDLs that boost the life- work in the blue to near-UV range due to problems
time exceeding 106 shots at a repetition rate of a few related to attenuation and photostability under UV ex-
Hz when pumped at 532 nm. Narrow-linewidth opera- citation, several UV laser dyes have been doped into
tion with a linewidth of 1.12 GHz has also been achieved sol-gel materials [11.1574, 1575]. Laser action with
in dye-doped MPMMA using a multiple-prism grating output wavelengths as short as 340 nm have been ob-
resonator cavity [11.1565]. Further improvement of the served [11.1575].
polymer host will undoubtedly lead to SSDLs that would From the recent development of polymer or sol-
gain the acceptance of the common laser users. gel dye lasers, one must rely on the role of materials
engineering in advancing solid-state dye lasers.
Solid-State Dye Lasers Based on a Sol-Gel Host
The sol-gel method is a low-temperature glass-making Distributed Feedback Waveguide Dye Lasers
technique that enables the introduction of organic dyes Distributed feedback (DFB) lasers are compact tunable
into inorganic glasses. Porous glass can be obtained laser sources that produce narrow-linewidth output. The
via the sol-gel route by hydrolysis and polyconden- first DFB laser was in fact a solid-state dye laser (dye-
sation of metal alkoxides [11.1568]. Initial studies of doped gelatin film), but it did not operate as a waveguide
sol-gel silica doped with organic dyes indicated that laser because of the high film thickness [11.1576]. In
sol-gel materials held good promise as SSDL host ma- subsequent developments, the majority of DFB laser
terials because of their wide transparency range and the work has concentrated on semiconductor lasers that
apparently excellent optical and thermal properties of have been of obvious industrial significance. Recently
silica [11.1559, 1569]. An added advantage is the high there has been a renewal of interest in organic DFB
concentration without aggregation and the photostabil- lasers, particularly those based on waveguide struc-
ity of a dye when trapped in sol-gel silica, as a result tures. This renewal in interest was caused in part by the
of the isolation of dye molecules in the silica cage. application of conjugated polymers as luminescent ma-
Soon tunable laser action from sulforhodamine-doped terials [11.1577, 1578] and the subsequent conjugated
sol-gel silica was demonstrated [11.1570]. Lasing and polymer laser experiments [11.1579, 1580]. Dye-doped
fluorescence properties of a large number of dyes in polymeric materials or sol-gel materials can be pre-
sol-gel silica that cover the spectral range from the near pared in a planar waveguide structure by simply using
ultraviolet to the near infrared were fabricated and ex- spin-coating or dip-coating. Sol–gel materials have the
amined [11.1571]. Several variants of sol-gel materials additional advantage of a larger range of refractive in-
have been used as solid-state dye-laser host materials dex variation [11.1581, 1582] which allows integrated
with varying degree of success. The first sol-gel mater- optics application on a large number of polymer or glass
ial used in dye-laser experiments was in fact a glassy gel substrates. DFB configuration seems ideally suited for
obtained by the gelation of a solution and is sometimes laser output generation in these waveguide structures.
called a xerogel [11.1572]. Xerogel derived from inor- Polymeric [11.1583] and sol-gel [11.1562] DFB wave-
782 Part C Coherent and Incoherent Light Sources

of the substrate surface. One of the interesting features


Dye-doped DFB
plastic array chip of DFB waveguide dye lasers is the possibility of the
LD-pumped microchip production of tunable multiple-wavelength output. Oki
Powell Nd: YAG laser (SHG)
lens et al. [11.1584, 1585] fabricated a multi-striped plastic
waveguide laser array that could generate multiple out-
put wavelengths in the range 575–945 nm (Fig. 11.183).
Another approach to obtain multiple output wavelengths
Part C 11.8

Cylindrical is to take advantage of waveguide structures that support


Laser lens
multiple propagation modes [11.1586]. Figure 11.184
Fig. 11.183 Schematics of Nd:YAG-microchip-pumped DFB dye shows the scan traces of a prism coupler for a titania–
lasers [11.1578] zirconia organically modified silicate waveguide on
a glass substrate [11.1587]. The titania–zirconia organ-
guide dye lasers with tunable narrow-linewidth output ically modified silicate film has a thickness of 6.7 µm
have indeed been demonstrated. and a refractive index of 1.56. Eight TE modes and
Figure 11.182 shows the typical setup for the gen- eight TM modes were observed. The action of the cross-
eration of a sol-gel DFB waveguide dye laser. The ing beams produced DFB laser output with wavelengths
dynamic grating responsible for the lasing effect was that obey the Bragg condition, λL = ηλp /M sin θ, where
produced by the crossing beams, which also served as η is the refractive index of the gain medium at λL , λp
the pump. Tuning was by varying the incident angle is the pump-laser wavelength, and M is the Bragg re-
of the beams and hence the grating period. The pe- flection order. For DFB laser action in waveguides, η
riodic perturbation necessary for DFB lasing can also takes on the values of the effective indices for TEi
be produced by permanent morphological modulation modes or TMi modes (i. e., i varies from 0 to 7 for
a 6.7 µm film). Figure 11.185 shows a typical DFB laser
output spectrum with a polarizer that blocks the TM
Intensity (arb. units)
modes [11.1587]. Without the polarizer all eight pairs of
400 TE/TM modes could be observed. It was found that the
crossing s-polarized beam generated purely TE modes,
TM whilst pairs of TE/TM modes were produced when p-
300 polarized beams were used. Furthermore, the separation
between the modes and the number of modes can be
controlled by varying the waveguide parameters such
200
Intensity (arb. units)
1

400

TE
300 0.5

200

0
53 52 51 50
Angle (deg) 560 580 600 620
Wavelength (nm)
Fig. 11.184 Scans of TE TM waveguide modes for a sol-gel
titania–zirconia organically modified silicate waveguide of Fig. 11.185 Output emission spectrum of a multiple wave-
thickness 6.7 µm and a refractive index of 1.56 on a glass length sol-gel DFB waveguide dye laser. The conditions of
substrate using a prism coupler the waveguide are the same as in Fig. 11.184
Lasers and Coherent Light Sources 11.8 Dye Lasers 783

as the index difference and guiding-film thickness. Si-


Wavelength (nm)
multaneous tuning of multiple output modes was also 610
achieved (Fig. 11.186). Such compact tunable multiple-
wavelength lasers should find wide applications from TE4
analytical spectroscopy to optical communications. TE3
600 TE5 TE2
Distributed Feedback Laser Action TE6 TE1

Part C 11.8
by Polarization Modulation TE7 TE0
The original DFB laser theory describes the laser action
caused by periodic perturbation of gain or refractive in- 590
dex [11.1576, 1588] both of which could be generated
by intensity modulation. A schematic of a typical cross-
ing beam experiment is illustrated in Fig. 11.187. The
580
two beams are shown to have their polarization direc-
tions at an angle Φ. The crossing beams must both be
s-polarized (Φ = 0◦ ) for the formation of an intensity
42 43 44 45
interference pattern (intensity modulation). The inten- Intersection angle (deg)
sity interference pattern in the gain medium produces
a concentration grating of excited-state atoms/molecules Fig. 11.186 Wavelength tuning of a multiple wavelength sol-gel
which will provide the periodic change in gain or re- DFB waveguide dye laser. The conditions of the waveguide are
fractive index necessary for DFB laser action. The the same as in Fig. 11.184
crossing of an s-polarized beam with a p-polarized beam
(Φ = 90◦ ), however, does not produce an intensity in- time the feedback mechanism was provided by polar-
terference pattern. Instead, a periodic change of the ization modulation. The distinguishing feature of DFB
polarization (polarization modulation) of the resultant lasing induced by the polarization modulation is the ap-
field that changes from linear polarization to elliptical pearance of a pair of TE0 /TM0 output modes, whereas
polarization to circular polarization and then back to el- only the TE0 mode is observed in the case of intensity
liptical polarization after one period. The grating that modulation.
results from polarization modulation is a polarization Our latest experiments on polarization modulation
grating. have revealed that DFB lasing can also be induced in
Figure 11.188 shows the DFB laser emission spec- liquid dye solution. The pump threshold is drastically re-
tra of rhodamoine 6G-doped zirconia waveguides as Φ duced by increasing θ. For θ larger than 75◦ , as is the case
changes from 0◦ to 90◦ for θ ≈ 44◦ [11.1587]. The pump for DFB lasing of liquid oxazine dye near 800 nm un-
energy used was 10 µJ. The situation at Φ = 0◦ corre- der the first-order Bragg condition, the threshold pump
sponds to the case of pure intensity modulation. The
variation of Φ changes the amplitude of the s-polarized
component of the beam. As Φ increases, the effective-
ness of intensity modulation weakens as the disparity
in amplitude of the s-polarized components of the two
crossing beams grows, resulting in a low degree of mod-
ulation in the transient intensity grating. At Φ = 60◦ , DFB output Sample DFB output
the amplitude of the electric field of the s-polarized O
component is 1/2 of the companion beam. The effect
of intensity modulation is already so weakened that 2è
Ö
a substantial ASE (attenuated spontaneous emission)
background (ratio of the DFB output intensity to the ASE
intensity of 10:3) appears in the emission spectrum. At S
Φ = 90◦ , DFB lasing is completely extinguished since
the s-polarized component of one of the beams has zero
amplitude. The pump energy was then gradually raised Fig. 11.187 Schematics for polarization modulation DFB
to about 30 µJ. DFB lasing reappeared at 30 µJ, but this laser experiments
784 Part C Coherent and Incoherent Light Sources

Intensity (arb. units) Intensity (arb. units)


1 1
TE0 TE0
Ö = 0° Ö = 60°

0.5 0.5
Part C 11.8

0 0

580 600 620 580 600 620


Wavelength (nm) Wavelength (nm)
Intensity (arb. units) Intensity (arb. units)
1 1
TE0
Ö = 80° Ö = 90°

0.5 0.5

0 0

580 600 620 580 600 620


Wavelength (nm) Wavelength (nm)
Intensity (arb. units)
1
TE0
Ö = 90°
3 times pump

0.5
TM0

580 600 620


Wavelength (nm)

Fig. 11.188 Output emission spectra of sol-gel DFB waveguide dye lasers as Φ varies

energy for DFB lasing by polarization modulation is the for many applications in optoelectronics. Many dyes
same as that by intensity modulation. Further work on (e.g., R6G, DCM) have been known to emit weakly
DFB lasing by polarization modulation is underway. in the visible when pumped in the near infrared. In-
deed, broadband laser emission in the visible was
Two-Photon-Pumped Solid-State Dye Lasers observed in two-photon pumped polymer waveguide
Compact visible lasers by direct upconversion of in- and fiber [11.1589, 1590]. A number of dyes with
frared light are versatile light sources that hold promise large two-photon pump upconverted absorption cross
Lasers and Coherent Light Sources 11.9 Optical Parametric Oscillators 785

Intensity (arb. units) Wavelength (nm)

1
Absorption 640
Fluorescence
ASE

0.5 620

Part C 11.9
1.06 µm pump M=3
M=2 1064 nm pump
600
0 532 nm pump
400 600 800 1000 1200
Wavelength (nm) 40 50 60 70
Intersection angle (deg)
Fig. 11.189 Absorption, two-photon-pumped fluorescence
and ASE spectra for an HMASPS-doped zirconia wave- Fig. 11.190 Tuning curves for DFB lasing in HMASPS-
guide doped zirconia waveguides

section have been synthesized recently. In particular, the pump, DFB lasing was observed in the red with
a styrylpyridinium dye: trans-4-[p-(N-hydroxyethyl- a linewidth as narrow as 45 GHz. Subsequent experi-
N-methylamino) styryl]-N-methylpyridinium p-toluene ments demonstrated tuning by varying the intersection
sulfonate (abbreviated as HMASPS) that shows strong angle of the two 1.06 µm crossing beams [11.1592].
emission in the red [11.1591] was doped in sol-gel Figure 11.190 shows the tuning curves for second
zirconia thin films on a glass substrate [11.1592]. Fig- (M = 2) and third (M = 3) Bragg orders. A tuning range
ure 11.189 shows the absorption, two-photon-pumped of 25–30 nm was observed. Extension of the spectral
fluorescence and ASE spectra from the HMASPS thin- coverage and improved output performance of the two-
film waveguides. A strong emission peak centered at photon-pumped DFB lasing are expected as more new
620 nm is seen. Using two crossing 1.06 µm beams as two-photon dyes are explored for DFB lasing study.

11.9 Optical Parametric Oscillators


Optical parametric oscillators (OPO) are based on non- Kroll [11.1599] and realized in 1965 by Giordmaine
linear frequency conversion of laser radiation into two and Miller [11.1600], followed by detailed theoretical
coherent light waves with lower frequencies, called the and experimental investigations [11.1601–1603]. Sev-
signal and idler waves. The first optical nonlinear con- eral review articles display a survey about the state of
version experiment was demonstrated soon after the the art of optical parametric oscillation until the mid
invention of the laser by the observation of second- 1980s [11.1604–1607].
harmonic generation of ruby laser radiation in a quartz However, despite this initial efforts, the success of
crystal [11.1593]. This first result initiated intense ex- OPOs as a versatile tunable light source fell short of ex-
perimental and theoretical investigations to increase pectations for almost a decade. At that time the reasons
the conversion efficiency and the available wavelength were unsuitable birefringence of the crystals to permit
range. In the following several years the physics of the phase matching, low transparency and damage thresh-
nonlinear frequency conversion was theoretically well olds, difficulties in growing large homogenous crystals
understood and all important methods of maximizing and the lack of reliable laser sources with good spatial
the conversion efficiency were elaborated, including and spectral properties, which are important for efficient
quasi-phase matching [11.1594, 1595], birefringence frequency conversion.
phase matching in crystals [11.1596, 1597] and the re- This situation changed due to significant advances
quirement for optimum focusing [11.1598]. The first in crystal growth techniques in the mid 1980s for both
optical parametric oscillator was proposed in 1962 by laser-active and nonlinear crystals [11.1608,1609], lead-
786 Part C Coherent and Incoherent Light Sources

ing to a renaissance of solid-state lasers. The availability medium. Because χ (2) is zero in centrosymmetric sys-
of reliable pump sources with high spatial and spectral tems three-wave mixing is only possible in non-isotropic
coherence (in continuous and pulsed operation mode), media. Generally, the χ (2) tensor possesses 27 elements,
low-loss optical components and the appearance of new but many of the components vanish under certain sym-
or optimized nonlinear materials (BBO, LiB3 O5 (LBO), metry conditions. The tensor can be reduced even to
KTiOPO4 (KTP), KNbO3 ) started a new OPO evolu- a scalar if the interacting waves are linearly polarized
tion. Optical parametric oscillators are powerful devices and monochromatic for a fixed crystal orientation. In this
Part C 11.9

for the efficient generation of widely tunable coher- case, the effective nonlinearity is denoted by a coefficient
(2)
ent light. The intense research in OPOs has resulted χeff . In the literature [11.1614] the second-order suscep-
in reliable OPO systems, which are commercially avail- tibility is often expressed by a coefficient d defined by
able. The tunability and the high output power define d := χ (2) /2.
the optical parametric oscillator as an attractive source The dynamics of optical parametric generation or
in many applications including high-resolution spec- three wave-mixing processes in general can be described
troscopy, environmental monitoring, medical research, by a set of nonlinear coupled differential equations for
process control, remote sensing and precision frequency the field amplitudes of the optical waves interacting with
measurements. the nonlinear medium.
Recently a new generation of conversion media Considering the basic wave equation derived from
have appeared with periodically structured ferroelec- Maxwell’s equations for nonmagnetic dielectric media
tric materials for quasi-phase matching. Together with where Pnl is regarded as source radiation
the development of diode-pumped all-solid-state lasers
and in particular high-brightness diode-laser systems d2 d2
∇ 2 E = µ0 ε E + µ0 Pnl (11.160)
new perspectives are opened towards modern, compact, dt 2 dt 2
efficient, powerful, tunable OPO systems. and assuming
∂E 1 (z)
11.9.1 Optical Parametric Generation = iκ1 E 3 (z)E 2∗ (z) ei∆kz , (11.161)
∂z
∂E 2 (z)
The theoretical treatment of optical parametric gener- = iκ2 E 3 (z)E 1∗ (z) ei∆kz , (11.162)
ation has been presented in the early 1960s [11.1610, ∂z
∂E 3 (z)
1611] and is found in many textbooks and review arti- = iκ3 E 1 (z)E 2 (z) e−i∆kz , (11.163)
cles [11.1604–1606,1612–1614]. Therefore, this section ∂z
will provide only a brief description of the most impor- with the coefficients κi = ωi deff /n i c0 (i = 1, 2, 3), deff
tant equations. The interaction of intense laser fields the nonlinear coefficient, z the propagation direction and
with a dielectric material induces nonlinear susceptibili- ∆k = k3 − k2 − k1 the phase mismatch.
ties and causes the polarization of the medium to develop This set of equations, the coupled wave equations
new frequency components not present in the incident represents the interaction of three plane waves in a χ (2)
radiation field. nonlinear dielectric. They have been solved exactly by
The lowest-order nonlinear susceptibility χ (2) is Armstrong et al. [11.1594] for various input conditions.
responsible for three-wave mixing processes such Depending on the initial conditions for the three complex
as second-harmonic generation (SHG), sum- and amplitudes, these equations describe the various types
difference-frequency mixing (SFG, DFG), optical rec- of three wave-mixing processes generated by the single-
tification and the optical parametric generation (OPG). pass propagation of the electromagnetic field through the
Optical parametric generation with a feedback resonator crystal, such as second-harmonic generation, sum- and
for at least one of the waves is called optical paramet- difference-frequency mixing and parametric generation.
ric oscillation (OPO). The relation between the electric The optical parametric generation process where
field E and the polarization density P in the medium is only one wave with frequency ω3 enters the dielec-
given for a second-order susceptibility as tric medium and generates two waves with the lower
P = ε0 (χ (1) E + χ (2) EE) frequencies ω1 and ω2 is based on the optical para-
metric fluorescence starting from the quantum noise.
P = Pl + Pnl (11.159)
This pure quantum mechanical effect was first pro-
with ε0 the vacuum permittivity and the susceptibility posed and studied in 1961 by Louisell et al. [11.1615].
χ (k) , which are tensors of the rank k for an anisotropic A quantum-mechanical model [11.1616] and semiclas-
Lasers and Coherent Light Sources 11.9 Optical Parametric Oscillators 787

sical descriptions of the optical parametric fluorescence In the low-gain limit where Γ 2l 2 < (∆k/2)2 the gain
can be found in the literature [11.1612, 1613, 1617]. of a parametric amplifier is
The process of parametric amplification starts with  1 
 ∆k 2
a small field amplitude of the signal (ω1 = ωs ) or idler sin2 2 − Γ 2 2 l
wave (ω2 = ωi ). The relation between the frequencies is G s (l) = Γ 2 l 2  2  . (11.170)
always ωs + ωi = ωp and per the definition ωs ≥ ωi . ∆k
− Γ 2 l
2
Introducing the definition for the intensity
Considering perfect phase matching ∆k = 0, the single-

Part C 11.9
I = 1/2ε0 nc|E|2 the coupled field equations lead to the
Manley–Rowe equation [11.1618] which is equivalent pass signal gain in the low-gain limit approximates to
to photon conservation. G s (l) ∼
= Γ 2l 2 ∝ d 2 l 2
eff (11.171)
dIs dIi dIp It can be seen that the magnitude of the parametric
= =− (11.164)
ωs dz ωi dz ωp dz gain depends on the intensity of the incoming field, as
well as on the material parameters such as nonlinear
The conversion of every pump photon generates a pair coefficient, refractive index and the interaction length.
of signal and corresponding idler photons. In this sense However, the main condition for an efficient parametric
the relation ωp = ωs + ωi corresponds to energy con- amplification is the phase-matching condition. As shown
servation and ∆k = kp − ks − ki = 0 to the impulse in Fig. 11.191 the parametric gain reaches a maximum
conservation of the parametric process. for ∆k = 0, and decreases symmetrically to zero for
Neglecting pump field depletion ( dE p / dz = 0) and |∆kl| = π.
assuming the presence of only the signal field (E i = 0) The gain bandwidth is defined by
in the beginning of parametric process the coupled wave   1/2
1 2
equations can be solved analytically [11.1605, 1606]. ∆k − Γ 2 l = π , (11.172)
The single-pass fractional gain in signal intensity is 2
obtained as which reduces for low gain to
 
Is (z = l) sinh2 gl 1
G s (l) = − 1 = Γ 2l 2 , (11.165) ∆kl = π . (11.173)
Is (z = 0) (gl)2 2
where l is the length of the nonlinear medium and g the The gain bandwidth increases with higher gain, but
total gain factor until reaching Γ 2 l 2 ∼
= π the bandwidth broadening is
 small.
 
∆k 2
g = Γ2− , (11.166)
2 sinc2 (Äk l/2)
and Γ the parametric gain factor 1.0

2ωs ωi |deff |2 Ip
Γ2 = . (11.167) 0.8
n p n s n i ε0 c3
The material-dependent part of the gain coefficient 0.6
FWHM = 0.88ð
|deff |2 /(n p n s n i ) is called the figure of merit (FOM)
and classifies the nonlinear quality of the conversion 0.4
medium.
In the high-gain limit the single-pass gain becomes 0.2
   
∆k 2 0
Gs = 1 + sinh2 gl (11.168) –2ð –ð 0 ð 2ð
2g Äk l

which reduces to Fig. 11.191 Parametric gain of a nonlinear crystal of length


l as a function of the phase mismatch ∆kl. The gain is
1
G s (l) ∼
= e2Γ l (11.169) maximum by optimum phase matching ∆kl = 0. The full
4 width at half-maximum (FHWM) of the gain function is
when ∆k < g. 0.88π
788 Part C Coherent and Incoherent Light Sources

11.9.2 Phase Matching


Intensity
As shown before effective three-wave-mixing in a non-
linear medium is only achieved if the phase-matching
condition (∆k = kp − ks − ki = 0) is fulfilled. Together
with the frequency-matching condition (ωp = ωs + ωi ),
this condition implies the spatial phase matching of the QPM
Part C 11.9

three waves which is necessary for constructive inter- BPM


ference of the interacting waves within the nonlinear
medium. NPM
This conservation of energy and momentum is not
0 1 2 3 4
possible in materials with isotropic dispersion. Due to Length (lc)
the different diffraction indices, the optical fields of the
three frequencies differ in phase velocity and the relative Fig. 11.192 Conversion intensity as function of the prop-
phase of the interactive waves varies along the medium. agation length in a nonlinear crystal. NPM: Non-phase-
A measure of the phase mismatch is the coherence length matched process with no significant total conversion
L c = π/|∆k|, which defines the distance over which intensity. BPM: birefringence phase matching. Intensity in-
the relative phase of the interacting waves shifts by π. 2
creases quadratically with z, with a slope given by deff,BPM .
The propagation beyond the coherence length, which is QPM: Quasi-phase-matched process. Intensity increases
typically several µm, leads to back-conversion from the quadratically with z on average, with a slope given by
generated waves into the pump wave. The oscillating 2
deff,QPM deff,BPM
2

behavior of the generated intensity depending on the


interaction length is shown in Fig. 11.192. cal solution of the phase matching angle is only possible
Today there are two different techniques to real- for type I phase matching in uniaxial crystals, the other
ize a phase-matched conversion process: birefringence processes have to be solved numerically [11.1609]. The
phase matching and the quasi-phase matching. analysis in biaxial crystals is more complicate and has
only numerical solutions; only in their principle planes
Birefringence Phase Matching can the formalism be reduced to the uniaxial condi-
This method uses the dependence of the refractive in- tions (Table 11.47 [11.1619, 1620]. A consequence of
dex on the propagation direction and polarization of angular birefringence phase matching is the spatial walk-
electromagnetic waves in birefringence crystals. The off generated by the birefringence, which reduces the
waves are distinguished into ordinary (o) and extraordi- interaction length of the optical waves. Besides the an-
nary (e) waves depending on their polarization direction. gular phase matching the indices of refraction can be
In uniaxial crystals the refractive index of the ordi- matched by changing the crystal temperature (temper-
nary wave is independent from the propagation direction ature phase matching). Combined with a propagation
whereas the refractive index of the extraordinary wave direction perpendicular to the principal axis this method
depends on the polar angle between the optical axis is called noncritical phase matching (NCPM) and re-
and the propagation direction. To achieve phase match- sults in the absence of spatial walk-off and less angular
ing the polarization of the high-frequency pump wave sensitivity, which is important in applications with tight
should be selected so that the index of refraction is focusing.
smallest. The phase-matching condition can be realized The vector equation of the phase matching condi-
by choosing an appropriate angle between propaga- tion can be realized in a non-collinear or a collinear
tion direction and optical axis. Angular phase-matched way. In contrast to the collinear phase matching is the
wavelength tuning is then possible by changing the non-collinear phase matching a vector phase matching.
phase-matching angle with regard to the phase-matching Figure 11.193 shows the non-collinear angle included
condition n p ωp = n s ωs + n i ωi . The process is called by the wavevectors. With the choice of a suitable non-
type I phase matching when both generated waves have collinear angle the angular acceptance is enlarged or
the same polarization perpendicular to the polarization the Poynting vector walk-off can be compensated. The
of the pump wave, for example (e–oo). For type II phase conditions for the walk-off compensation are shown
matching the polarization of the generated waves are in Fig. 11.193a; the Poynting vectors of the ordinary
oriented perpendicular to each other (e–oe). An analyti- signal and the extraordinary pump wave are paral-
Lasers and Coherent Light Sources 11.9 Optical Parametric Oscillators 789

Table 11.47 Refraction indices of ordinary and extraordinary wave for uniaxial and biaxial crystals in the principle planes
Crystal Extraordinary wave (e) Ordinary wave (o)
no n e
Uniaxial n e (Θ) =  n o (Θ) = n o
n 2e cos2 Θ+n 2
o sin
2

xy nx n y
Biaxial, xy-plane n e (Φ) =  n o (Φ) = n z
n 2x cos2 Φ+n 2y sin2 Φ
nx nz
e (Θ) =
n xz n o (Θ) = n y

Part C 11.9
Biaxial, xz-plane 
n 2x cos2 Θ+n 2z sin2 Θ
yz n y nz
Biaxial, yz-plane n e (Θ) =  n o (Θ) = n x
n 2y cos2 Θ+n 2z sin2 Θ

lel. Such walk-off compensation is of advantage for for a long time. Recent advances in the fabrication
nanosecond OPOs reaching higher conversion efficien- of structured ferroelectrics meanwhile have estab-
cies [11.1621] and necessary for critical-phase-matched lished this technique for efficient frequency-conversion
OPOs pumped by ultrashort pulses because of the small applications.
beam radii [11.1622, 1623]. The diagram of tangential Quasi-phase matching through periodically pol-
phase matching is shown in Fig. 11.193b. This special ing offers two major advantages over birefringence
case of non-collinear phase matching produces a signif- phase matching. First, the polarization of the in-
icant enlarged angular acceptance for the extraordinary teracting waves can be equal. This allows the use
pump wave. In addition, group-velocity matching for of the largest χ (2) coefficient of the crystal, which
ultrashort pulses is realized via non-collinear phase reduces the pump threshold and increases the con-
matching [11.1624]. version efficiency. The second advantage is that the
quasi-phase matching of any combination of pump,
Quasi-Phase Matching signal and idler wavelength can be realized in such
An alternative method to achieve phase matching materials via periodic poling. In addition, QPM pro-
via phase correction is quasi-phase matching (QPM). vides design flexibility of nonlinear conversion devices
Here the relative phase between the three waves is by engineered domain structures. Applications with
corrected using a periodic change in the sign of novel configurations such as chirped gratings for
the nonlinear susceptibility (Fig. 11.192) before the pulse compression [11.1625], fan-out gratings for
back conversion starts. Although the technique of broad tunability [11.1626], quasi-periodic structures
QPM was proposed even before birefringence phase for simultaneous operation of two three-wave-mixing
matching [11.1594], difficulties in fabrication of the pe- processes [11.1627] and two-dimensional gratings for
riodic structure in the range of the coherence length multiple direction phase-matching processes [11.1628]
(typically 1–100 µm) have prevented its realization have been demonstrated.

a) Principal axis b) Principal axis

S3 S3

S3 k2

k2
k3
k3
k1
Fig. 11.193a,b Wavevector diagram
k1 Non–collinear
for different non-collinear phase-
Non–collinear angle matching schemes. (a) Walk-off
angle compensation, (b) scheme for tan-
gential phase matching
790 Part C Coherent and Incoherent Light Sources

Phase Mismatch and Acceptance Bandwidths photon is converted into a signal and idler photon fulfill-
The ideal phase-matched interaction, where the pump ing photon-wise energy conservation ωp = ωs + ωi . The
wave and idler and signal waves propagate with the resonator feeds the signal wave back into the crystal
same velocity through the nonlinear crystal, ∆k = 0, where it is further amplified through the power transfer
is affected under real experimental conditions by sev- from the pump wave, as expressed in (11.164). Optical
eral parameters such as the divergence and bandwidth parametric oscillation starts, when the increased signal
of the pump radiation, the bandwidth of the generated intensity surpasses threshold that means the amplified
Part C 11.9

radiation and an inhomogeneous temperature distribu- signal wave compensates for the round-trip losses in
tion. The tolerances of the nonlinear material concerning the resonator (due to mirror transmission, absorption,
to these perturbations are expressed by the acceptance scattering and diffraction). Reaching this distinct pump
bandwidths. They are defined by the FWHM of the para- intensity, the threshold pump intensity, a significant por-
metric gain width (Fig. 11.191) and developed in Taylor tion of the pump intensity is converted into signal and
series of ∆k(0): idler intensity. This power transfer from the pump to the
Angular acceptance generated waves reduces the (spatially averaged) pump
intensity inside the nonlinear crystal and thus the sig-
∆δ = 2 × 0.886πl −1 (δ∆k/δδ)−1 ; nal gain. This effect is called gain saturation. It leads
Gain band width to steady-state operation of the OPO, where the signal
∆ωs = 2 × 0.886πl −1 (δ∆k/δωs )−1 ; power generated inside the crystal exactly balances the
resonator losses for the signal wave.
Spectral acceptance As any pair of signal and idler photon can be gener-
∆ωp = 2 × 0.886πl −1 (δ∆k/δωp )−1 ; ated from the initially random vacuum field fluctuations
Temperature acceptance in steady-state operation, the signal and idler frequency
pair that has the minimum threshold pump intensity
∆T = 2 × 0.886πl −1 (δ∆k/δT )−1 . (11.174) is generated. Thus the generated frequencies, and with
them the ratio of the signal and idler frequency, are de-
11.9.3 Optical Parametric Oscillators termined by the frequency dependence of the parametric
gain in the crystal and the frequency dependence of the
An optical parametric oscillator consists of three basic resonator losses.
components, namely the pump source, the gain medium, A detailed description of the behavior of optical
and the feedback resonator. For a qualitative description parametric oscillators has been published in several
of the operation principle we consider the most basic reviews [11.1604–1606] and the physics of OPOs is
OPO setup, as shown schematically in Fig. 11.194. discussed more fundamentally in a number of textbooks
An intense coherent light field produced by a laser about nonlinear optics [11.1612–1614].
beam propagates through an optically nonlinear crystal In the literature, optical parametric oscillators are
with the frequency ωp . The crystal is placed inside an mostly classified into three groups: continuous-wave op-
optical resonator, which resonates for reasons of sim- tical parametric oscillators, nanosecond pulsed optical
plicity with one wave, for example the signal wave. parametric oscillators and synchronously pumped pi-
As the nonlinear crystal provides a sufficient nonlin- cosecond or femtosecond optical parametric oscillators,
earity, parametric generation takes place and a pump depending on the temporal characteristic of their pump
laser.
This distinction is not only a practical classification
Nonlinear
crystal but is important for the theoretical description and the
íp ís
basic performance, such as pump intensity at threshold,
Pump source
íi
conversion efficiency and spectral performance.
M1 M2
11.9.4 Design and Performance
Fig. 11.194 Schematic setup of an OPO. An optical wave of Optical Parametric Oscillators
with frequency νp from the pump source is converted into
two output waves with frequencies νs and νi via three-wave The performance of an optical parametric system con-
interaction in a nonlinear crystal. M1 and M2 are mirrors cerning tunability, high output intensity, spectral and
of a feedback resonator spatial coherence is directly related to key elements
Lasers and Coherent Light Sources 11.9 Optical Parametric Oscillators 791

of the OPO’s architecture, which are pump source, the available pump power is restricted the OPO design
nonlinear material and feedback resonator. In general, may have to be modified for lower threshold, which
the physics of the optical parametric process imposes might however restrict the tuning capabilities of the
several requirements of potential OPO components. OPO. Three types of feedback resonators are distin-
A simultaneous optimization of all OPO features guished, depending on the number of resonating waves.
cannot be fairly done because of material problems and The singly resonant OPO (SRO) has highly reflecting
physical conflicts. Therefore, a general description of mirrors at the signal or the idler wave. In principle, this

Part C 11.9
an optimized OPO design is not possible and the device configuration is of particular advantage because it should
configuration is always a compromise depending on the provide continuous wavelength tunability. The disad-
requirements of the specific application. vantage of these systems are their high pump power at
The choice of the pump laser depends together with threshold, which exceeds several watts [11.1629, 1630].
the selection of the nonlinear material on the required Therefore SRO devices are mainly found for pulsed OPO
wavelength range and time resolution for a given ap- configurations.
plication. Obviously, the pump laser has to be powerful Doubly resonant OPO configurations (DRO) where
enough to drive the OPO well above threshold and guar- both signal and idler waves are resonated have received
antee stable OPO operation. Since good spatial and much attention, because the pump power at thresh-
spectral beam quality reduces the threshold, preferred old is reduced by one to three orders of magnitude.
pump sources will be high-power lasers of several watts, However, such DRO OPOs do not provide mode-
which also provide an excellent spatial beam quality, hop-free tunability and often suffer from frequency
and good power and frequency stability. If the available and power instabilities [11.1631, 1632]. Continuous
pump power is restricted, low beam divergence is of par- wavelength tuning requires active stabilization tech-
ticular importance to allow focusing into the nonlinear niques [11.1633, 1634].
crystal. The deviations in spectral and spatial coherence The doubly resonant configuration where pump
tolerated by the parametric frequency conversion are de- and signal (or idler) waves are resonated is called
termined by the acceptance bandwidths of the nonlinear pump-enhanced SRO (PESRO). Such devices are very
material. Wavelength tunability of the pump laser offers attractive because they provide a compromise between
an additional attractive feature: tuning of the OPO via the low pump power at threshold of DROs and the
the pump wavelength. wide tunability of SROs when the length of the OPO
The selection of the nonlinear material depends is carefully locked to a frequency-stabilized pump
on the nonlinear parametric process, the experimental laser [11.1635]. In addition, a continuous tunability is
design and the properties of the pump source. Funda- possible with a pump-enhanced SRO, by using a res-
mentally, the nonlinear crystal should be distinguished onator internal beam splitter to separate the pump
by a broad transparency range, a high optical-damage spatially from the resonated OPO wave [11.1636]. These
threshold and large effective nonlinearity. An important waves are then resonated on two separate cavity end
parameter is the birefringence of the crystal that has mirrors (dual cavity) for independent control of the
to be high enough to maintain phase matching. How- resonated OPO wave and the length of the pump cavity.
ever, this effect should not be too large because another Triply resonant OPOs (TRO) suffer from the com-
consequence of birefringence is spatial walk-off, which bined problems of both types of DROs, consequently
reduces the interacting length of the coupled fields. they provide less tunability in comparison to SRO and
Large spectral and angular acceptance bandwidths are DRO, but they are remarkable because of their low
advantageous because real laser systems show finite threshold pump power in the range of several mW or
bandwidths and divergence and in ultrashort optical below [11.1637, 1638].
parametric oscillation, the temporal walk-off and group-
velocity dispersion between pump, signal and idler wave Continuous-Wave Optical Parametric Oscillators
should be low. For stable operation of OPO systems with Continuous-wave optical parametric oscillators (CW-
high energies the thermo-mechanical and thermo-optical OPOs) are efficient and highly coherent light sources
stability of the crystal should be sufficient. Finally, the in the near- and mid-infrared. Due to their tunability,
crystals should be available in appropriate dimensions these sources are of considerable interest for high-
and excellent optical homogeneity. resolution spectroscopy of molecules and trace-gas
The design of the feedback resonator is strongly con- detection [11.1639]. Simplified and improved frequency
nected to the output characteristic of the pump source. If standards are currently being considered, based on the
792 Part C Coherent and Incoherent Light Sources

strong frequency and phase correlation of the OPO’s With Γ 2lc2 = αι αs the pump intensity at the DRO
signal and idler output waves [11.1640, 1641]. threshold is similarly derived as
After the first demonstration of CW OPOs in 1968  
αi αs n p n s n i −2 ∆klc
by Smith et al. [11.1601] and Byer et al. [11.1602] sig- Ip,th = sinc . (11.178)
4 ωs ωi deff
2 l2
c 2
nificant progress is this field was made in the beginning
of the 1990s, supported by advances in crystal growth A low threshold is achieved when a long nonlinear
techniques [11.1609], low-loss optical components and crystal with a high figure of merit is used inside a sig-
Part C 11.9

CW solid-state lasers. nal resonator with highly reflecting mirrors. In general


As discussed before pump power at threshold de- the pump threshold is lower for higher signal and idler
creases with increasing cavity finesse for each of the frequencies. However, via the sinc function of the phase
wavelengths. Typical values for the pump power at mismatch the pump threshold is exposed to an additional
threshold are listed in Table 11.48 for CW OPOs with and much stronger dependence on the signal and idler
the different resonators (TRO, DRO, SRO). wavelength. A minimum threshold is achieved for signal
The pump power at threshold of singly resonant and idler wavelengths with ∆k = 0. As a consequence
OPOs is significantly higher than 1 W, even in a high- the OPO always seeks to oscillate as close as possible to
finesse cavity with no significant output coupling of the phase-matched wavelengths.
the resonant wave. Since most commercially available Usually CW OPOs are pumped with focused
single-frequency lasers provide maximum pump pow- beams to enhance the pump power, therefore pump,
ers of about 1 W, most CW OPOs demonstrated in the idler and signal waves are expressed as Gaussian
past are doubly or triply resonant devices. beams [11.1644]. In this case the intensity shows an
The threshold pump intensity can be calculated from inhomogeneous distribution along the propagation axes
the coupled wave equations in analogy to the parametric z and the intensity and phases are not constant within
gain assuming all three waves (pump, signal and idler) each of the xy-planes. Only for loose focussing can
are infinite plane waves, with uniform intensity across these inhomogeneities be neglected and is equation
the beam, neglecting focusing and double refraction. (11.177) still a good estimation of the pump intensity
The gain is considered to be unidirectional and the pump at threshold. The pump power at threshold for tight fo-
depletion is always small at threshold. cussing has been derived in an detailed mathematical
At the steady-state threshold, the gain balances treatment [11.1614, 1645], which is beyond this scope.
the resonator losses for each resonator round-trip. The For optimized confocal focussing [11.1598], the pump
threshold condition for an SRO is power at threshold is given by
E s (0) = (1 − αs )E s (lc ) . (11.175) 4πc2 n s n i αs
Pp,th = . (11.179)
Where αs are the round-trip losses of the resonant µ0 ωs ωi ωp deff
2 l
c
signal wave and lc is the crystal length. In the low-gain As opposed to the lc−2 dependence of the threshold in-
limit and assuming small losses, the parametric gain tensity for plane waves (11.177) for the pump power
coefficient (11.167) can be written [11.1606] of Gaussian beams decreases linearly with the crystal
length.
Γ 2 lc2 = 2αs . (11.176)
Once above threshold a part of the pump power Pp is
Then we obtain the pump intensity at the SRO converted into the appropriate signal and idler waves as
threshold long as the effective gain is larger than one. An impor-
  tant parameter is the pump depletion, which occurs until
npnsni −2 ∆klc
Ip,th = αs sinc . (11.177) the gain is saturated and the steady state is reached.
ωs ωi deff
2 l2
c 2
The analytical description of the internal conversion
efficiency ηint can be obtained under steady-state condi-
Table 11.48 Typical pump power at threshold for CW TRO, tions assuming small cavity losses and optimum phase
DRO, SRO matching. The conversion efficiency
OPO Pump threshold (mW) Ref. Pout,p
ηint = 1 − (11.180)
TRO <1 [11.1633] Pin,p
DRO 100 [11.1642]
depends on the ratio of the incoming and the transmit-
SRO 2600 [11.1643] ted pump power and is a function of the pump ratio
Lasers and Coherent Light Sources 11.9 Optical Parametric Oscillators 793

N0 (N0 = Pp /Pp,th ) [11.1645]. The maximum conver- One of the most crucial components of CW OPOs
sion efficiency for plane waves comes to 100% for is the nonlinear material. For successful CW OPO op-
a pump ratio of N0 = (π/2)2 . The extension of this eration it is of particular importance that the crystals
model to Gaussian intensity distributions with plane nonlinearity is high and noncritical phase match-
wavefronts yields maximal conversion efficiency of 71% ing is possible. Crystals used so far are noncritical
supposing a pump ratio of 6.5. The conversion efficiency phase-matched LiNbO3 , KTP, LBO, Ba2 NaNb5 O15
is reduced by the inhomogeneous intensity distribu- and KNbO3 whereas especially KTP and its arsenate

Part C 11.9
tion of the pump wave as well as distortions of the isomorphs KTiOAsO4 (KTA) and RbTiOAsO4 (RTA)
wavefronts. turned out to be attractive materials for CW OPOs.
Due to parasitical losses in the cavity (Fresnel losses Wavelength tuning of NCPM OPOs requires either
at the surfaces, diffraction and absorption), the measured temperature tuning of the crystal or wavelength tun-
output power is lower than predicted by the internal ing of the pump laser. Because of the low-temperature
efficiency. Therefore, it is useful to determine an external tuning capability of the KTP crystal family wave-
(utilizable) conversion efficiency, which in steady-state length tuning in such OPOs depends on tunable pump
conditions is sources. Many investigations have been performed with
T ωs DROs and pump-enhanced OPOs to achieve continu-
ηext,s = η, (11.181) ous tunability. A significant increase of the continuous
T + L ωp
tuning range was realized with the dual-cavity de-
assuming small transmission T of the output mirror and sign [11.1634,1636,1652]. Low-threshold operation has
small losses L for the resonant signal wave. been demonstrated with a TRO and pump-enhanced
In order to operate the CW OPO continuously SRO KTP OPO pumped with a single-stripe GaAlAs
with low fluctuations in output power and frequency, diode laser [11.1652, 1653]. High idler powers of
the cavity length needs to be stabilized. The main 840 mW in the wavelength range of 2.4–2.9 µm have
sources of cavity length fluctuations are thermally in- been achieved with KTP and KTA OPOs designed
duced fluctuations of the refractive index, mostly in the as an intracavity SRO configuration and pumped by
crystal, and acoustically and thermally induced pertur- Ti:sapphire lasers [11.1654]. An important step was the
bations of the position of the cavity mirrors. Fluctuations realization of a singly resonant CW OPO [11.1629].
caused by these sources are usually significant just In recent years the availability of novel quasi-phase-
for low-frequency ranges, i. e., ν < 10 kHz, which can matched nonlinear material and high-power solid-state
be compensated, for example, by an electronic sta- lasers enabled significant advances in the development
bilization device. (For higher-frequency components, of CW OPOs. The high optical nonlinearity of periodi-
i. e., ν > 10 kHz, the noise of the pump laser is sig- cally poled LiNbO3 (PPLN) and long interaction lengths
nificant instead of the cavity length fluctuations). For up to 50 mm enables the operation of CW SROs pumped
an OPO with pump enhancement resonance, a change by CW solid-state lasers. Pumping such a 50 mm-long
of the cavity length induces a mismatch between the PPLN crystal with the 13.5 W output of a high-power
cavity resonance frequency and the pump laser fre- diode-pumped Nd:YAG laser, infrared radiation tunable
quency, resulting in an increased OPO threshold and in the range of 3.25–3.95 µm with an output power of
decreased output power. If the OPO is resonant for the 3.6 W has been reported [11.1655]. The measured pump
signal or the idler wave or for both simultaneously, the depletion was as high as 93%. Wavelength tuning was
change of the cavity length leads to fluctuations of the achieved through temperature tuning or by using differ-
signal and idler frequencies and to mode hops and clus- ent poling periods implemented on the crystal. A step
ter hops. One possible method to stabilize the cavity toward compact efficient and powerful CW OPOs was
length is to increase the passive stability in a monolithic performed with the realization of a diode-laser-pumped
setup [11.1646]. However, pump-enhanced OPOs and singly resonant PPLN OPO [11.1656]. The SRO con-
doubly resonant OPOs usually require active control of sists of a 38 mm-long PPLN in a four-mirror cavity
the cavity length [11.1647]. To stabilize a cavity reso- (Fig. 11.195). Pumping with 25 W of 925 nm laser radi-
nance to a laser frequency several methods have been ation from an AlGaAs master-oscillator power-amplifier
successfully demonstrated [11.1648–1650]. Long-term (MOPA) system, 480 mW of single-frequency idler ra-
stabilization of a doubly resonant parametric oscillator diation was generated. The tuning range of the idler
where the frequency instability is below 1 kHz has been covers 2.03–2.29 µm. In addition several investigations
demonstrated [11.1651] have been performed with pump-enhanced SROs in
794 Part C Coherent and Incoherent Light Sources

M1 M2 Filters OPO wavelength (nm)


Diode 2200
MOPA PPLN
iso Idler
L
2100

M3 M4 2000
460 nm
Part C 11.9

Fig. 11.195 Experimental setup of the diode laser pumped


1900 Idler
singly resonant OPO (SRO). The pump beam from the 2.1 K
MOPA system propagates through a 60 dB isolator (iso) Signal
1800
and focuses into the PPLN crystal. All mirrors of the ring
cavity are highly reflecting for the signal wave and highly
1700
transmitting for the pump and idler wave. The idler output
behind M2 is filtered from the residual pump and signal 1600
radiation by dielectric filters [11.1656] 147 148 149 150
Crystal temperature (° C)

PPLN. Tunable radiation was generated in the range Fig. 11.196 Temperature tuning curve of a near-degenerate
of 2.29–2.96 µm with an output power of 140 mW PPLT OPO calculated for a pump wave of 925 nm and
pumped by 800 mW delivered from a miniature diode- a grating period of 27.3 µm [11.1660]. Shaded areas: para-
pumped single-frequency Nd:YAG laser [11.1657]. An metric gain bandwidth of the 35 mm long PPLT crystal at
extension of the wavelength into the mid-IR between degeneracy is as large as 460 nm. The Sellmeier coefficients
4.07–5.26 µm was demonstrated by pumping a PPLN can be found in [11.1661]
PESRO by CW single-frequency Ti:sapphire radia-
tion [11.1658]. Another pumping design was performed parison between the performance of PPKTP and PPLN
using a high-power fiber laser. The Yb-doped fiber laser was performed within these investigations [11.1664].
generated in a 40 mm-long PPLN crystal mid-IR idler These cited examples clearly indicate the dynamic in
powers in the range 2.98–3.7 µm. Pumping with 8.3 W this field. Further research in new ferroelectrics generat-
laser power the OPO generated 1.9 W [11.1659]. ing radiation beyond 5 µm and the improvement of the
Besides the successful demonstration of powerful existing materials concerning dimensions, homogeneity
PPLN OPOs one severe disadvantage of PPLN is the and structure design will lead to high-efficiency compact
appearance of photorefractive effects, which may dam- integrated optical systems.
age the crystal. Some effort is made to optimize the
growing technique in such a way that these defects can Nanosecond Optical Parametric Oscillators
be avoided. Optical parametric oscillators pumped with nanosecond
Other QPM materials have also been developed, pulses are the most well-established OPO systems gen-
such as periodically poled KTP (PPKTP) [11.1662– erating powerful tunable radiation in the spectral range
1664], RTA (PPRTA) [11.1665] and Lithium tantalate from the visible to the near infrared. Since the first
(PPLT) [11.1660]. Due to the high purity of these ma- demonstrated optical parametric oscillator [11.1600],
terials photorefractive defects do not occur even at high which was a nanosecond pulsed OPO, reliable nanosec-
pump levels. ond OPOs were not established before the late 1980s.
Wide wavelength tunability has been reported in the The appearance of new nonlinear materials with large
range 1.5–4 µm in PPLN [11.1666] and 1.55–2.3 µm nonlinearity and high damage thresholds (larger than
in PPLT[11.1660] pumping the OPOs near degeneracy, 1 J/cm2 ) such as BBO, LBO, and the improvement of
which provides large parametric gain bandwidths for the optical quality of KTP or KNbO3 was the start of
a given poling period, crystal temperature and pump an intense OPO evolution. These materials together with
wavelength (Fig. 11.196). In PPLT the wavelength tun- the optimized spatial beam quality and high peak powers
ing is achieved by changing the crystal temperature of modern nanosecond Q-switched lasers made it pos-
within an interval of only 10 K. Operating a CW OPO sible to reach the threshold of the single-resonant OPO
with subsequent frequency-doubling wavelength tun- configuration.
ability from the visible to the mid-IR range between The basic principle of optical parametric oscillation
550–2830 nm has recently been demonstrated. A com- for nanosecond OPOs is the same as for CW oscilla-
Lasers and Coherent Light Sources 11.9 Optical Parametric Oscillators 795

tors; however, due to the finite length of the pump pulse the length of the crystal. The threshold identifies the de-
(typical pulse lengths are 2–30 ns) the OPO does not tectable level of the signal energy, which corresponds to
reach the steady-state regime. In nanosecond OPOs, the an energy of typical 100 µJ, giving a threshold power to
cavity length is about a few centimeters, which corre- noise ratio of ln(Pth /Ps ) = 33. The time required from
sponds to less than 100 round-trips for the pump pulse. the parametric gain of the signal field starting from the
The steady-state threshold is no longer valid because noise level P0 to reach the oscillation threshold Pth is
of the transient character of pulsed OPOs. The dy- called the rise time of the parametric oscillator. The

Part C 11.9
namic behavior was considered in a model developed rise time is an important parameter in the design and
by Brosnan and Byer [11.1667] using a time-dependent operation of a parametric oscillator and can be cal-
gain analysis. They calculated the buildup to threshold culated from the time-dependent coupled amplitudes
for a signal resonant optical parametric oscillator by equations. For efficient conversion, the rise time has
assuming a Gaussian temporal profile for the incident to be as short as possible. Pearson et al. [11.1668]
pump pulse intensity and a Gaussian spatial distribu- carried out a detailed investigation of the rise time as
tion for the pump and the signal beams. Additionally a function of various experimental parameters, such as
their model assumes single pass of the pump wave pump pulse length, cavity length, cavity losses and the
and considers the effects of mode overlap and spatial pump ratio N0 , which is the factor between the pump
walk-off. pulse energy and the pump pulse energy at threshold,
They introduced the time-dependent parametric gain N0 = Pp /Pp,th . Important experimental parameters to
coefficient Γt minimize the rise time are high pump energy densities
and a short cavity length. Beyond the influence of the
√ ω2p
gs Γ e−( τ )
t 2
Γt = with gs = , rise time the threshold energy density can be reduced
ωp + ω2s
2
by using long pump pulse durations τ, optimizing the
(11.182) reflectivity R and avoiding intracavity losses α. Addi-
tionally the nonlinearity of the crystal should be large
where τ is the 1/ e2 intensity half-width of the Gaussian and the length of the crystal should be as long as pos-
pump pulse. The spatial coupling efficient gs describe sible with regard to the limitation through the Poynting
the mode overlap between the resonant signal wave and vector walk-off.
the pump wave. The influence of the Poynting vector The spectral bandwidth of a singly resonant opti-
walk-off defines the effective parametric gain length Λ cal parametric oscillator depends primarily on the gain
√ 
π lc bandwidth, which is determined by the dispersion, the
Λ = lω erf (11.183) birefringence and the length of the nonlinear crystal.
2 lω
In addition, the bandwidth is determined by the spec-
with the walk-off length, which depends on the birefrin- tral properties of the resonator, the correlation between
gence angle ρ, the resonator modes and the characteristics of the pump

√  laser, the wavelength, spectral bandwidth, intensity and
π ω  ω2p + ω2s divergence. Because of the short pump pulse duration
lω = . (11.184)
2 ρ ω2p + ω2s /2 for nanosecond pumped OPOs there is only a weak
spectral-mode condensation and the nanosecond OPO
The threshold energy fluence for the single-resonant does not reach the stationary state, unlike the CW OPO.
OPO is derived from the coupled wave equations, as- Usually the nanosecond OPO bandwidth is estimated
suming low pump depletion, as with the gain bandwidth, as there is no exact analytical
2.25 description of the spectral bandwidth of pulsed OPOs.
Jth = τ Neglecting any saturation Brosnan and Byer [11.1667]
κgs Λ2
 2 deduced an expression for the spectral condensation
lr Ps,th 1 depending on the number p of cavity round-trips
× ln + 2α2 lc + ln √ + ln 2
2τc Ps,0 R 1
(11.185) ∆ν( p) = √ ∆ν . (11.186)
p
2ω ω d 2
with κ = n ns n i εeffc3 , whereR is the reflectivity of the A more exact prediction concerning the theoretical
p s i 0
mirrors, α2 are the internal losses of the resonant wave bandwidth can be calculated using numerically simu-
inside the crystal, lr is the optical cavity length and lc is lations [11.1669, 1670].
796 Part C Coherent and Incoherent Light Sources

Nanosecond pulsed optical parametric oscillators are the crystal for wavelengths longer than 2600 nm. The
powerful devices of widely tunable coherent light. With pump energy density at threshold is about 200 mJ/cm2 .
the nonlinear crystals BBO and LBO such OPOs pro- Pumped with 2–10 ns-long pulses such OPO devices op-
vide coherent radiation in the entire spectral range from erate routinely with conversion efficiencies in the range
the UV (300 nm) to the near IR (2.5 µm). The advan- of 20–50% whereby the optical damage threshold of the
tageous properties of these crystals are high optical OPO components limits the pump ratio. The spectral
damage threshold, high nonlinearities, a wide trans- bandwidth of the type I phase-matched 355 nm-pumped
Part C 11.9

parency range and a large birefringence. Since the first BBO OPO varies from 0.2 nm in the blue spectral
successful operation of a BBO OPO reported by Fan range (λ = 400 nm) to more than 10 nm at degeneracy
et al. in 1989 [11.1671] significant progress in OPO tech- (λ = 710 nm). The spectral bandwidth of the idler wave
nology has been achieved. In the investigations reported equals (expressed in wavenumbers or GHz) that of the
so far, BBO OPOs have been pumped with the second, corresponding signal frequency.
third, and fourth harmonics of a Q-switched Nd:YAG In the past, many efforts have been made to re-
laser at 532 nm [11.1671,1672], 355 nm [11.1672–1677] duce the spectral bandwidth of OPOs. Significant line
and 266 nm [11.1672, 1678], and with the fundamental narrowing, even to single-mode operation, can be
of an XeCl excimer laser at 308 nm [11.1679,1680]. The achieved with the insertion of frequency selective el-
highest output energies and efficiencies have been ob- ements (such as gratings or etalons) into the OPO
tained with the third harmonic of Q-switched Nd:YAG resonator or with external injection seeding of the OPO.
laser. The generated output energies are in the range Although these methods can provide single-mode oper-
100–200 mJ/pulse and external conversion efficiencies ation, the disadvantages are obvious. First, the addition
of up to 61% have been reported [11.1672, 1681]. of frequency-selective elements increases the resonator
Similar advances have been demonstrated for length, the cavity losses and thus the oscillation thresh-
the LBO OPO that covers almost the same spec- old. Therefore, higher pump densities are required and
tral range [11.1669, 1682–1688]. The power densities a compromise is needed between the necessary pump
at threshold for the 355 nm-pumped LBO OPO are power and the damage threshold of the optical compo-
typically higher by a factor of two compared to nents. Second, continuous wavelength tuning may be
those of equivalent BBO OPOs due to the lower affected by the complexity of such devices. The spec-
effective nonlinear coefficient. However, LBO pos- tral line narrowing via injection seeding avoids these
sesses a smaller spatial walk-off angle than BBO disadvantages; the threshold is even reduced, because
[ρ(LBO) ≈ 0.25ρ(BBO)] allowing the use of longer of a shorter rise time [11.1690]. Nevertheless, success-
LBO crystals to compensate the lower nonlinearity. The ful injection seeding in pulsed OPOs depends on many
experimental comparisons of LBO and BBO [11.1669, fundamental parameters of the OPO operation. Besides
1686] demonstrate the advantageous properties of LBO proper collinear alignment and divergence adaptation
as there are large angular acceptance, low spatial walk- between the seed radiation and the seeded OPO wave,
off (which can even be zero for temperature-tuned the frequency matching between the cavity mode and
noncritical phase matching). These properties are valu- the seed frequency is essential. Despite these difficulties
able if the OPO is to be operated with low-pump-energy successful line narrowing was demonstrated with both
laser sources (< 3 mJ) [11.1689], whereas BBO with methods [11.1675, 1681, 1691–1693]. A theoretical de-
restricted angular acceptance and larger nonlinearity scription of the spectral characteristic of free-running
is more suitable for high-pump-energy laser sources or injection-seeded OPO systems are given in several
(> 100 mJ). numerical models [11.1669, 1670, 1694, 1695].
In the past many investigations were performed pri- The investigation and the control of the spatial beam
marily for the type I critically phase matched BBO quality of nanosecond OPOs is still a challenge. As a re-
OPO pumped by the third harmonic of a Nd:YAG laser. sult of large pump-beam diameters, high nonlinear gain
This well-established standard OPO consists typically of in the crystal and a large Fresnel number of the optical
a 12–15 mm-long BBO crystal placed in a linear signal resonator the beam quality factor M 2 of the generated
resonant Fabry–Pérot resonator. Changing the phase- radiation are often high > 2–10 and thus far from the
matching angle in the range of 10◦ the OPO covers diffraction limit (M 2 = 1). Most of the numerical models
a tuning range of 400–710 nm for the signal wave and simulating the spatial behavior of nanoseconds OPO are
710–3100 nm for the idler wave. Experimentally the time integrated [11.1696–1699]. Recently time-resolved
idler tuning is restricted by an increase of absorption in experimental and numerical investigation of the spec-
Lasers and Coherent Light Sources 11.9 Optical Parametric Oscillators 797

tral and spatial dynamics of nanosecond OPO has been ficiencies up to 40%, generating output powers of about
reported [11.1700, 1701]. The result of the different in- 5 W or pulse energies of 5 mJ [11.1716, 1717]. The dif-
vestigations is, that the OPO starts on the optical axis ficulty of finding the appropriate pump lasers for these
with an almost Gaussian beam profile. However, during materials has been overcome with cascaded OPO sys-
the buildup of the pulse the fields undergo an inhomoge- tems published for AgGaSe2 and CdSe [11.1717–1720].
neous gain caused by the birefringence walk-off in the A new generation of nanosecond OPOs appeared
OPO crystal, pump depletion and back-conversion and with the availability of periodically poled QPM ma-

Part C 11.9
as consequence the M 2 value increases with the size of terials as there are PPLN, PPKTP, PPKTA and
the pump energy, pump depletion and back-conversion. PPRTA. These crystals have large effective nonlinear-
Some investigations of the spectral and tempo- ities (8–16 pm/V), up to eight times higher than in
ral dynamics of the OPO has been performed using a corresponding BBO crystal, and possess long in-
a BBO OPO, which consists of a 2–3 mm-long crys- teraction lengths. Typically the aperture of the QPM
tal in a 3.5 mm-long cavity [11.1670, 1701]. Due to the crystals are 1 mm high. Therefore, these materials
wide mode spacing of about 1 cm−1 each single mode are well suited for the generation of mid-IR radi-
can be considered. Figure 11.197 shows the statisti- ation pumped with high-repetition low-power-pump
cal mode fluctuation of 10 successive pulses. Thus, the pulses [11.1721–1723]. With the development of wide
short-cavity OPO proofs the macroscopic manifestation large-aperture PPRTA crystals, QPM becomes suitable
of the zero-point fluctuation of the vacuum. also for high-power applications [11.1724, 1725]. The
Based on the numerical and experimental results large nonlinearity of PPLN enables the operation of effi-
some improvement on the spectral and spatial perfor- cient single-pass optical parametric oscillators [11.1721,
mance of nanosecond OPOs were developed based on 1726–1728]. More recently tunable single-frequency
novel pumping and resonator configurations [11.1621, generation has been demonstrated with injection-seeded
1702–1708]. PPLN OPOs and PPLN OPGs [11.1729–1731].
For the generation of wavelengths up to 5 µm the ap-
propriate crystals are KTP, KTA and KNbO3 [11.1709– Synchronously Pumped Optical Parametric
1712]. Further extension to wavelengths beyond Oscillators
5 µm can be achieved in ZnGeP2 , CdSe and Optical parametric oscillators synchronously pumped
AgGaSe2 [11.1713–1717]. Avoiding two-photon ab- by mode-locked solid-state lasers are powerful devices
sorption in the materials these crystals have to be for the generation of tunable ultrashort laser pulses. The
operated with pump wavelengths longer than 1.5 µm. first CW synchronously pumped picosecond OPO was
Meanwhile nanosecond OPOs are demonstrated with demonstrated by Piskarskas et al. in 1988 [11.1732] and
a tuning range up to 14 µm. They provide conversion ef- the first synchronously pumped femtosecond OPO by
Edelstein et al. in 1989 [11.1733].
Many reports of such OPOs generating pulses in
the picosecond or femtosecond regime have been pub-
lished in recent years [11.1734–1736]. Ultrafast laser
systems are attractive pump sources for optical paramet-
ric oscillators. They combine high peak pulse intensities
providing sufficient nonlinear gain with a moderate en-
ergy fluence preventing optical damage of the material.
However, remembering the instantaneous character of
nonlinear polarization the optical gain is obtained exclu-
sively during the time interval of the pump pulses length.
In contrast to nanosecond OPOs, the time interval of ul-
trashort pulses (τ < 100 ps) is too short to allow a finite
549.8 550 550.2
Signal wavelength (nm)
number of cavity round-trips. Therefore, the basic oper-
ation principle of ultrafast optical parametric oscillators
Fig. 11.197 Mode spectra of the signal wave (550 nm) is synchronous pumping to achieve macroscopic ampli-
recorded for 10 successive OPO pulses. The OPO is op- fication of the parametric waves from quantum noise.
erated at 1.44 times above threshold. The mode spacing is In this pumping scheme the length of the optical para-
28.8 GHz (0.96 cm−1 ) [11.1670] metric oscillator is matched to that of the pump laser
798 Part C Coherent and Incoherent Light Sources

resonator, so that the round-trip transit time in the OPO


resonator corresponds to the repetition time of the pump
pulses. The consecutive coincidence of parametric and l3
M3 M4
pump wave in the nonlinear crystal amplifies the gain
l2 Pump
until it overcomes the threshold.
In general, two types of synchronously pumped á
C M2
OPOs are to be distinguished: the pulsed (or quasi- l1
Part C 11.9

CW) synchronously and the continuous synchronously


pumped OPOs. CW synchronously pumped OPOs are
M1
pumped with a continuous train of ultrashort pulses as
they are emitted by CW mode-locked neodymium lasers Fig. 11.198 Experimental setup for a linear standing wave
or Kerr lens mode-locked Ti:sapphire lasers, while the resonator consisting of two plane mirrors M1 and M4 and
pump sources of pulsed synchronously pumped OPOs two spherical mirrors M2 and M3. The pump laser beam is
are mode locked Q-switched Nd lasers generating a train focused into the crystal C between the spherical mirrors M2
of ultrashort pulses contained within a nanosecond or and M3. The total resonator length depends on the distance
microsecond envelope. between two successively pump pulses
The physical description of CW synchronously
pumped OPOs is equivalent to the steady-state for- length of 1.85 m. The tolerance of the resonator length
malism for CW OPOs considering the peak pump detuning can be calculated from ∆lres = ∆τ(c/2), which
pulse intensity determining the nonlinear gain. Pulsed is half the geometrical pump pulse length. The theo-
synchronously pumped OPOs show the transient be- retical detuning calculated for 1 ps is about 150 µm,
havior of nanosecond OPOs so their analysis has to however experimentally even shorter detuning toler-
take into account the rise-time effects caused by the ances of 30 µm are affordable.
finite time duration of the nanosecond pulsed enve- Commonly used resonator designs for syn-
lope [11.1667]. An analysis of synchronously pumped chronously pumped OPOs are ring or standing-wave
OPOs can be found for plane-wave conditions [11.1737] resonators, where the latter is favorable for compactness
and for Gaussian beams in CW synchronously pumped reasons (its length is half that of the ring). A typi-
OPOs [11.1738, 1739]. cal standing-wave resonator for synchronously pumped
Most of the early synchronously pumped OPOs were OPOs is shown in Fig. 11.198 consisting of two plane
pulsed OPOs [11.1734] because of the significant higher and two spherical mirrors.
peak pump pulse powers compared to CW mode-locked
pump lasers at that time. Picosecond optical parametric Picosecond optical parametric oscillators. Picosecond
oscillation even in the SRO configuration was gen- optical parametric oscillators synchronously pumped by
erated using the nonlinear materials KTP [11.1740], CW mode-locked solid-state lasers are powerful devices
BBO [11.1622] and LBO [11.1741]. However due to for the generation of tunable ultrashort laser pulses es-
the pulsed pump characteristic the output of such OPOs pecially in the IR spectral region. For many applications
does not consist of a really repetitive pulse train, and in high-resolution spectroscopy a high spectral inten-
the amplitude, intensity and the pulse duration of the sity and a narrow bandwidth is required. As the light of
output pulse can vary under the pulse envelope. In ap- such OPOs is almost Fourier limited (15 ps = 1 cm−1 )
plications where no high peak powers are needed CW picosecond pulses (with t > 10 ps) have a sufficient se-
synchronously pumped OPO are advantageous because lectivity for spectroscopy, in contrast to pulses in the
of their continuous train of output pulses. Meanwhile femtosecond regime. Similar to the nanosecond pulsed
with the availability of efficient CW mode-locked lasers OPOs the high peak powers of modern CW mode-locked
and more-reliable nonlinear materials the research in this lasers easily overcome the threshold of SRO resonators.
field is focused on CW synchronously pumped OPOs. As a consequence, most synchronously pumped CW
In practice, synchronously pumping is a reason- OPOs operate in the SRO configuration.
able pumping mechanism only for high repetition rates In the past, there have been various ways to generate
(> 50 MHz) otherwise the resonator length becomes too tunable picosecond IR radiation by CW synchronously
long and unpractical. For example, typical repetition pumped OPOs. In most synchronously pumped pi-
rates of Kerr lens mode-locked Ti:sapphire lasers are cosecond OPOs, the use of noncritical phase matching
about 80 MHz, which corresponds to an OPO resonator prevents a reduction of interaction length due to walk-off
Lasers and Coherent Light Sources 11.9 Optical Parametric Oscillators 799

between the focused beams inside the nonlinear crystal. wave, are summarized in experimental investigations for
Wavelength tuning of noncritical OPOs requires a varia- picosecond and femtosecond radiation [11.1748, 1749].
tion of the pump wavelength or the crystal temperature. High-power operation of a singly resonant pi-
A temperature-tuned picosecond LBO OPO has cosecond OPO has been reported pumping a critical-
been reported [11.1742] generating continuously tun- phase-matched KTP OPO with the fundamental of an
able radiation between 650 nm and 2.5 µm with a single mode-locked Nd:YLF laser at 1.053 µm [11.1750]. This
crystal. The average output power achieved by this sys- device generates 12 ps-long signal pulses at 1.55 µm for

Part C 11.9
tem was below 100 mW. By using tunable pump laser 40 ps-long pump pulses at a repetition rate of 76 MHz.
systems like the Kerr-lens mode-locked Ti:sapphire A total average output power of 2.8 W was achieved
laser pump wavelength tuning offers a convenient tuning with 800 mW in the idler wave at 3.28 µm.
mechanism. The new generation of mode-locked lasers are
A noncritical-phase-matched picosecond KTP OPO diode-pumped CW mode-locked Nd:YVO4 oscillator–
[11.1743] generates tunable picosecond pulses in amplifier laser systems. Such an all-solid-state laser
the spectral ranges of 1–1.2 µm for the signal and system operating at 1.064 µm with 7 ps pulse lengths at
2.3–2.9 µm for the idler wave via wavelength tuning of repetition rates of about 83 MHz delivers average output
the pump between 720–853 nm. Average output powers powers of 29 W. Pumping a noncritical-phase-matched
of up to 700 mW in 1.2 ps pulses has been achieved with KTA OPO the OPO output power reaches the multiwatt
a pump power of 1.6 W at a 82 MHz repetition rate. region providing a signal wavelength of 1.53 µm with
The combination of wavelength tuning of the an output power of 14.6 W and an idler output power as
Ti:sapphire laser and temperature tuning in LBO high as 6.4 W at 3.47 µm in the mid-IR [11.1751]. The
has been performed under the type I noncritical- total average output power of 21 W corresponds to an
phase-matching condition, providing continuously tun- external efficiency of 70%. However, both systems op-
able picosecond pulses in the spectral range of erate at a specific signal and idler wavelength without
1–2.4 µm [11.1744]. The pump power was 1.2 W in any tunability.
1–2 ps pulses at a 81 MHz repetition rate and generated With the availability of QPM nonlinear materials like
an average OPO output power of about 325 mW. Using PPLN, PPKTP, PPRTA new perspectives have arisen
the arsenate isomorphs of KTP, such as KTA and RTA, in the research of efficient tunable picosecond OPOs.
the wavelength range of the OPO can be extended up to With the advantageous properties of these materials as
3.6 µm [11.1745]. Due to their wider transparency range their large nonlinearities, transparency in the mid IR and
and the lack of grey tracking inside the crystal these the capability to choose an optimized phase-matching
materials are advantageous for IR picosecond OPOs. condition for the interacting waves, for example non-
Further extension of the tuning range of picosecond critical phase matching, they become ideal candidates
OPOs into the mid-IR was demonstrated with a critical- to realize singly resonant synchronously pumped OPOs
phase-matched AgGaS2 OPO pumped by a Q-switched with low thresholds, large tunability and efficient out-
mode-locked Nd:YAG laser [11.1746]. This OPO had put powers. Compact all-solid-state devices have been
an idler tuning range of 3.5–4.5 µm and a maximum reported based on PPLN and PPRTA with a pump
output power of 2 W. power threshold as low as 10 mW [11.1752, 1753]. The
Picosecond pulse generation in the visible spectral generated radiation covers the wavelength range from
range has been demonstrated in an LBO OPO pumped 3.35–5 µm with total output powers of up to 400 mW
with the third harmonic of a CW mode-locked Nd:YLF in 1–5 ps pulses. The power of the idler wave was
laser [11.1747]. The generated output power was about up to 100 mW. The spectral range of the PPLN OPO
275 mW in the spectral range of 453–472 nm in 15 ps- has been extended even beyond 5 µm [11.1754] and
long pulses at a repetition rate of 75 MHz. idler output powers of 0.5 mW are achieved. The op-
In general, it should be pointed out that the de- eration of a PPLN OPO at GHz repetition rates was
vice Ti:sapphire-laser-pumped KTP or KTA OPO is demonstrated by pumping the PPLN OPO with an
a versatile tool for the generation of tunable picosec- all-solid-state neodymium laser at 10 GHz [11.1755].
ond pulses in the entire spectral region from the UV Rapid wavelength access was achieved with the use
to the near-IR. The frequency-conversion schemes in- of a mode-locked diode laser master-oscillator power-
volved, such as second, third, and fourth harmonics amplifier (MOPA) system providing 7.8 ps pulses at
of the Ti:sapphire laser, optical parametric oscillation 2.5 GHz repetition rate. The InGaAs oscillator–amplifier
in KTP and frequency doubling of the OPO’s signal system delivered an output power of 900 mW, which was
800 Part C Coherent and Incoherent Light Sources

converted to 78 mW idler power tunable in the spectral availability of the Kerr-lens mode-locked Ti:sapphire
range of 2.2–2.8 µm [11.1756]. laser. The first material used in synchronously pumped
A high-power picosecond PPLN-OPO was per- femtosecond OPOs was KTP [11.1763–1765] in
formed by synchronously pumping a PPLN crystal with non-collinear critical-phase-matching conditions and
the fundamental wave of a CW mode-locked Nd:YLF collinear noncritical-phase-matching condition. Due to
laser. The tuning range of the PPLN OPO is for the sig- the higher transmission in the mid-IRA OPOs with
nal radiation 1.765–2.06 µm and 2.155–2.61 µm for the KTA [11.1766, 1767], RTA [11.1768], CsTiOAsO4
Part C 11.9

idler radiation, respectively. High average output powers (CTA) [11.1769, 1770], and KNbO3 [11.1771] gener-
for the signal and idler radiation of 2.55 W and 2.4 W ate a wider wavelength range of 1–5 µm with pulse
have been achieved in 45 ps-long pulses at a 76 MHz durations of less than 100 fs. Typical maximum output
repetition rate for an input pump power of 7.4 W, which powers of such devices are 100–200 mW for the signal
corresponds to a total external conversion of about 67%. and 50–100 mW for the idler wave.
The measured pump depletion was 71% [11.1757]. The periodically poled nonlinear materials PPLN,
Much emphasis is placed on further extension of PPRTA, and PPKTP are of particular importance for
the tuning range of picosecond systems into the IR. femtosecond OPOs because noncritical phase match-
For this purpose OPO/OPA and OPG/OPA devices are ing becomes possible even for the extended wavelength
of great interest [11.1758, 1759] as their output pow- tuning. This feature results in compact, low-threshold,
ers and tuning ranges are sufficient to be used for efficient OPO devices. The wavelength tuning of such
difference-frequency mixing into the mid-IR. The differ- femtosecond QPM OPOs is performed via grating, pump
ence frequency mixing in GaSe or CdSe [11.1760–1762] wavelength or cavity tuning and covers the spectral range
of signal and idler frequencies generated from an PPLN from 1.7–5.4 µm in PPLN [11.1772], 1.06–1.22 µm
OPO seeded KTP-OPA provides picosecond pulses tun- (λs ) and 2.67–4.5 µm (λi ) in PPRTA [11.1773], and
able at 3–24 µm. 1–1.2 µm in PPKTP [11.1774]. Comparing these QPM
materials, PPLN and PPRTA have an advantage because
Femtosecond optical parametric oscillators. Tunable of their large transmission range, where PPLN possesses
femtosecond OPOs are attractive light sources for the higher nonlinearity. However PPLN suffers from
time-resolved spectroscopy of chemical and biological process-induced photorefractive defects, which may be
reactions. Femtosecond pulses are characterized by their suppressed by heating the crystal to temperatures higher
high peak powers, which easily overcome the threshold than 100 ◦ C. Recently MgO-doped PPLN-OPO was in-
of a singly resonant OPO configuration. The short pulse vestigated [11.1775] allowing reliable OPO operation at
length of about 100 fs is combined with a huge spectral room temperature.
bandwidth of several nanometers (≈ 10 nm) and disper- Tunable radiation in the range of 4–8 µm have been
sion effects, such as group velocity dispersion, group achieved using a cascaded AgGaSe2 OPO, which has
velocity mismatch (i. e., temporal walk-off) and spec- been pumped with the idler of a CTA OPO. This system
tral acceptance bandwidths can no longer be neglected. generates average powers of 35 mW in 300–600 fs-long
The group-velocity dispersion causes a pulse broaden- pulses at a repetition rate of 82 MHz.
ing whereas the temporal walk-off lowers the nonlinear Moreover, optical parametric generators and ampli-
gain and/or changes the time characteristic of output fiers are powerful tools for the generation of ultrashort
pulse. For efficient frequency conversion, the temporal pulses into further infrared regions [11.1776]. The gen-
walk-off has to be minimized by an appropriate choice eration of femtosecond pulses in the spectral range
of the crystal length. Typical crystal lengths of fem- 3–12 µm with almost bandwidth limited pulses of
tosecond OPOs are only 1–2 mm, and therefore high 100–200 fs have been reviewed for different parametric
nonlinearities are desirable for low operation thresholds. processes and a number of relevant materials [11.1777].
The group velocity dispersion can be minimized via dis- Many new perspectives for the generation of intense
persion compensation in the OPO cavity. Additionally ultrashort pulses are given by parametric amplification
to these dispersion effects, other higher-order nonlin- of chirped laser pulses. The basic principle of opti-
ear effects come with the high peak pump powers, such cal parametric chirped pulse amplification (OPCPA) is
as self-phase modulation and cross-phase modulation that stretched linearly chirped pump pulses are ampli-
which result in a chirped OPO output pulse [11.1613]. fied in a non-collinear phase-matched OPA. After the
The start of an extensive development of fem- single-pass amplification, the pulses are compressed,
tosecond OPOs was initiated with the commercial providing high energy in short pulse lengths of 10 fs
Lasers and Coherent Light Sources 11.10 Generation of Coherent Mid-Infrared Radiation by Difference-Frequency Mixing 801

or less. The non-collinear phase-matching scheme is to non-collinear phase matching but can be obtained
important because of the huge spectral bandwidths of at practically any center wavelength in the crystals
femtosecond pulses. For ideal OPCPA the pump pulse transparency window. Additionally QPM OPA can be
duration corresponds to the length of the chirped pulse. increased by using engineered grating profiles, such as
The spatial beam profile should be rectangular (flat-top), chirped gratings [11.1625], fanned gratings [11.1626],
and the gain should be constant temporally and spatially. and aperiodic gratings [11.1786].
Dubietis et al. [11.1776] published the first proposal Nondegenerate OPCPA has been demonstrated in

Part C 11.10
and demonstration of OPCPA. The first experimental PPKTP at a wavelength of 1573 nm pumped by
demonstrations of OPCPA were performed in degener- a Nd:YAG laser [11.1787] and close to degeneracy
ate LBO, KDP and BBO [11.1778–1782]. Amplification at a wavelength of 1053 nm pumped by a Nd:glass
of 1010 have been achieved in single-pass amplification laser [11.1788].
at degeneracy. This chapter describes the basic properties and cur-
The use of non-collinear phase matching enables rent performance of CW, nanosecond and ultrashort
the efficient parametrical amplification of nondegenerate optical parametric oscillators. Today these parametric
wavelengths despite large spectral bandwidth. Recently systems are powerful tunable light sources providing
different sources of supercontinuum have been ampli- a spectral range from the visible to the mid-IR in all
fied in BBO and other crystals via frequency-doubled time regimes. The main progress in this field is based on
Ti:sapphire lasers with 1 kHz repetition rate [11.1783, the development of more-sophisticated optical materials
1784]. Ultrashort pulses below 6 fs have been gener- and efficient, reliable laser systems. With the realization
ated, however the achieved pulse energies was lower of QPM materials there was an important breakthrough
than 5 µJ. towards compact widely tunable OPOs. Especially for
The generation of higher energies is possible by em- CW OPOs, QPM materials are the key element for
ploying visible picosecond pump pulses and temporally the realization of widely tunable singly resonant OPOs.
stretched seed pulses. At a center wavelength of 800 nm The high nonlinear gain of QPM materials enables the
and a pump wavelength of about 530 nm in BBO and reduction of the optical parametric oscillation to opti-
LBO gain bandwidths broader than 2000 cm−1 are ob- cal parametric generation, which leads to more-simple
tained, which is sufficient to amplify Fourier-limited devices. The combination of diode-pumped solid-state
pulses with 5 fs duration [11.1778]. Due to the large laser systems and QPM crystals, which already leads
damage thresholds of both materials, high pump inten- to direct diode-pumped OPOs, is the way to future,
sities can be applied. Recently OPCPA was performed compact tunable laser systems that may be realized in
at 800 nm and with a Nd:YAG laser at 532 nm, gener- integrated designs.
ating a gain of 4 × 106 in two BBO crystals [11.1785]. Finally it should be mentioned that, besides the
The pulse energy was 2 mJ at a 10 Hz repetition rate. importance of the generated OPO radiation for many
QPM materials also turn out to be advantageous in spectroscopic and technical applications, the OPO itself
OPCPA. Broad-bandwidth amplification is not restricted is still an interesting physical system to be explored in
any longer to collinear phase matching at degeneracy or the field of quantum mechanics.

11.10 Generation of Coherent Mid-Infrared Radiation


by Difference-Frequency Mixing
The fundamental infrared (IR) or mid-IR region of the depicted in the center. In view of applications in air mon-
electromagnetic spectrum between, say 3–20 µm, is of itoring the (relative) transmission through the terrestrial
special interest for many applications, notably molecular atmosphere is plotted at the bottom of Fig. 11.199.
spectroscopy [11.1789]. The reason is that most organic This atmospheric absorption is obviously dominated
and inorganic molecules exhibit strong vibrational– by the presence of water vapor and CO2 . The atmo-
rotational transitions in this wavelength region. This is spheric windows at 3–5 µm and 8–14 µm are clearly
illustrated in Fig. 11.199, where the absorption ranges visible.
of some important functional groups of molecules are In addition to the ultraviolet–visible and the near-IR
plotted for wavelengths of 2–20 µm (top), whereas range, the mid-IR region has attracted a lot of interest
absorption features of a few selected molecules are in recent times owing to the numerous applications of
802 Part C Coherent and Incoherent Light Sources

tunable laser source is a prerequisite for successful


Wavelength (µm) trace-gas sensing and analysis. In addition to tunability,
20 10 6 5 4 3.5 3 2.5 2
a narrow line width guarantees sufficient specificity of
Alkane detection in multicomponent real-world gas mixtures.
Alkene In the preferred mid-IR range, the choice of coherent
Alkyne/allene
Aromatic homocyclic
sources is, however, rather limited. Table 11.49 lists
Alcohol/phenol tunable lasers with wavelengths longer than 3 µm. It
Part C 11.10

Ethers essentially includes the conventional well-established


Organo-sulphur line-tunable CO and CO2 gas lasers, continuously tun-
Organo-halogen able semiconductor lasers (lead-salt diode and quantum
Organo-phosphorus cascade lasers), color center lasers, novel crystalline
solid-state lasers and nonlinear optical devices [optical
parametric oscillators (OPOs) and difference-frequency
generation (DFG) sources].
Recent progress both in solid-state lasers and
in quantum cascade lasers (QCLs) appears promis-
ing. Solid-state laser materials such as Ce2+ :ZnSe or
Fe2+ :ZnSe offer tuning ranges of 2.2–3.1 µm [11.1790]
: CO2 : NO2 : SO2 : O3 : NH3 : CH4 or 4–4.5 µm, respectively (though the latter only when
Transmission pulsed and with cryogenic cooling) [11.1791]. New
developments in QCLs equipped with external cavi-
CO2
ties yield a continuous tuning range of around 10%
of the central wavelength and – at least partly –
room-temperature continuous-wave operation [11.1792,
CO2 1793]. Despite these attractive prospects the broad-
est tuning range, best wavelength coverage, room-
H2O H2O temperature operation and highest flexibility in terms of
wavelength selection is currently still achieved with non-
500 1000 1500 2000 2500 3000 3500 4000 4500 5000
linear optical devices (DFG and OPOs) [11.1794]. Here
Wavenumbers (cm–1)
we focus on DFG as the scheme that has been widely
Fig. 11.199 Absorption ranges of important molecular functional used in recent times to access mid-IR wavelengths for
groups (top) and of selected molecules (center). The size of the sym- trace-gas sensing. In fact, these important applications
bols is related to the absorption strength. Atmospheric transmission have fostered further developments of DFG systems.
is depicted at the bottom
11.10.1 Difference-Frequency Generation
trace-gas sensing in rather diverse fields including en- (DFG)
vironmental monitoring and climate research, industrial
and process surveillance, workplace safety, agriculture Difference-frequency generation (DFG) represents
(e.g., ethylene or ammonia detection, surveillance of fer- a nonlinear optical effect that is related to the nonlinear
mentation), homeland security (e.g., chemical warfare susceptibility of second order (χ (2) ) of a material. Other
or explosives detection) and medical diagnosis (e.g., hu- related effects are second-harmonic generation (SHG)
man breath monitoring). It has been demonstrated in and sum-frequency generation (SFG). Hence, DFG rep-
numerous cases that laser spectroscopy offers the poten- resents a three-beam interaction process that is mostly
tial for high sensitivity and selectivity, multicomponent used to generate tunable coherent mid-infrared radiation,
capability, and large dynamic range. These are all cru- although it has also been employed for THz generation.
cial properties for trace-gas sensing. An important aspect
of laser-based sensors is that usually no sample prepa- Birefringent, Quasi-Phase Matching
ration, i. e., neither pretreatment nor pre-concentration, and Conversion Efficiency
are required, in contrast to many competing techniques. In difference-frequency generation the light of two laser
Apart from an appropriate detection scheme, which en- beams is mixed in a nonlinear crystal and light with
ables sensitive absorption measurements, a mid-infrared a frequency of the difference of the two incident fre-
Lasers and Coherent Light Sources 11.10 Generation of Coherent Mid-Infrared Radiation by Difference-Frequency Mixing 803

Table 11.49 Tunable continuous-wave mid-IR laser sources with wavelengths ≥ 3 µm. RT: room temperature, LN2 :
liquid nitrogen (77 K), TE: thermoelectric cooling, SHG: second-harmonic generation, QCL: quantum cascade laser,
OPO: optical parametric oscillator, DFG: difference-frequency generation
Laser Wavelength (µm) Tuning characteristics Power Operation
CO 5–6 (2.7 – 4, overtone) only line tunable 50 mW to W LN2 cooling, also ≤ 0 ◦ C
CO2 9–11 (4.5–5.5, SHG) only line tunable W RT operation
≈ cm−1 mode hop-free < 0.1 mW

Part C 11.10
Lead salt diode 4–30 Cryogenic cooling
QCL 4–> 24, THz cm−1 to > 100 cm−1 per device mW LN2 /TE cooling, also RT
Color center 1–3.3 ≈ 0.5 µm for single crystal 100 mW LN2 cooling
Solid-state 2.2–3.1 ≈ 0.5–1 µm ≤ 1W RT operation
OPO 3–16 ∼ µm for specific setup ≤ 1W RT operation
DFG 3–16 ∼ µm for specific setup µW to mW RT operation

quencies is generated. The generated frequency is given s, and i corresponding to pump, signal and idler, re-
by energy conservation: spectively, and c is the speed of light in vacuum. Phase
matching in a birefringent crystal can be achieved by
ωp − ωs = ωi → ωi = ωp − ωs . (11.187)
1. angle tuning
The laser with the highest frequency ωp is called the 2. temperature tuning
pump laser, while the second laser is called the signal 3. wavelength tuning (changing the wavelength of the
laser with a frequency ωs . The generated idler beam has pump and/or signal laser).
the lowest frequency ωi . The phase-matching condition
is given by the conservation of momentum: The most common way to achieve phase matching with
a birefringent crystal is realized by angle tuning, i. e., by
∆k = kp − ks − ki = 0 , (11.188) rotating the crystal until the phase-matching condition
where ∆k is the phase mismatch, and kp , ks , and ki are is fulfilled.
the wavevectors of the pump, signal, and idler beam, re- For infinite plane waves the idler intensity is given
spectively. In the case of collinear wave propagation the by [11.1795]:
wavevectors can be replaced by |k| = nc/λ and (11.188)  
ω2 d 2 L 2 Is Ip ∆kL
changes to: Ii = 2 i3 eff sinc2 (11.190)
c ε0 n p n s n i 2
np ns ni
− − =0, (11.189) where deff is the effective nonlinear coefficient, L is the
λp λs λi
crystal length, I is the intensity of the laser beam for
where n is the refractive index at the corresponding pump, signal and idler beams, respectively, ε0 is the di-
wavelength, λ is the wavelength with the subscripts p, electric constant, and ∆k is the phase mismatch. Hence
the idler intensity scales with the product of the incident
Table 11.50 Different phase matching types for DFG pro- intensities Is Ip and the square of the crystal length L 2 .
cesses for positive and negative birefringent crystals. PM: This is valid as long as there is no pump depletion and
phase matching, e: extraordinarily polarized, o: ordinarily negligible walk-off between the beams. These effects
polarized, QPM: quasi-phase matching limit the useful crystal length and they are discussed
PM Birefringence Pump Signal Idler in more detail in the section on nonlinear crystals. The
type beam beam beam effective nonlinear coefficient deff describes the non-
I Positive o e e
linearity of the crystal seen by the incident light and
depends on the crystal structure, the direction of propa-
I Negative e o o
gation, the polarization of the light, and the nonlinear
II Positive o e o
coefficients dij (Table 11.51) given by the tensor of the
II Negative e o e
nonlinear susceptibility χ(2) = 2d.
III Positive o o e
To achieve phase matching it is taken advantage of
III Negative e e o
the different refractive index for ordinarily and extraor-
QPM e e e dinarily polarized light. Depending on the combination
804 Part C Coherent and Incoherent Light Sources

Table 11.51 Nonlinear coefficients dij measured at wavelength λm , transparency range and approximate damage threshold
for ns pulses of selected nonlinear optical crystals used in DFG
Crystal Nonlinear coefficients (pm/V) [11.1796] λm Transparency Damage threshold
(µm) range (µm) pulsed (MW/cm2 )
[11.1797] [11.1797, 1798]
AgGaS2 d14 = 57 d36 = 20 10.6 0.46– 13 25
Part C 11.10

d36 = 23.6 1.064


AgGaSe2 d36 = 33 10.6 0.7–19 25
Ba2 NaNb5 O15 d31 = 12 d32 = 12 d33 = 16.5 1.064 0.37– 5 4
[11.1797] [11.1797] [11.1797]
CdGeAs2 d36 = 235 10.6 2.4–18 20– 40 [11.1799]
CdSe d15 = 18 d31 = −18 d33 = 36 10.6 0.57– 25 60
[11.1800] [11.1800]
CsTiOAsO4 (CTA) d31 = 2.1 d32 = 3.4 d33 = 18.1 1.064 0.35– 5.3 500 [11.1801]
GaAs d14 = 368.7 d36 = 83 10.6 1–17 [11.1799] 60 [11.1799]
[11.1800]
GaSe d22 = 54.4 10.6 0.62– 20 30
HgGa2 S4 d36 = 26 d31 = 6.7 1.064 0.55– 13 60
[11.1797]
KNbO3 d15 = −17.1 d24 = −16.5 d31 = −18.3 1.064 0.4–> 4 180
d32 = −15.8 d33 = −27.4
KTiOAsO4 (KTA) d31 = 4.2 d32 = 2.8 d33 = 16.2 1.064 0.35– 5.3 1200
d24 = 2.9
[11.1800]
KTiOPO4 (KTP) d15 = 1.91 d24 = 3.64 d31 = 2.54 1.064 0.35– 4.5 150
d32 = 4.53 d33 = 16.9
LiB3 O5 (LBO) d24 = 0.74 d31 = 0.8–1.3 d33 = 0 1.064 0.155– 3.2 900
d15 = 1.03 d24 = −0.94 d31 = 1.09 1.079
d32 = −10 d33 = −0.94
LiIO3 d15 = −5.53 d31 = −7.11 d33 = −7.02 1.064 0.28– 6 120
LiInS2 d31 = 9.9 d32 = 8.6 d33 = 15.8 10.6 0.35– 12.5 [11.1802] 100 [11.1802]
LiNbO3 d31 = −5.95 d33 = −34.4 1.064 0.4–5.5 [11.1803] 300
d33 = −27
[11.1800]
d31 = −5.77 d33 = −33.4 1.150
d31 = 3.77 d33 = −31.8 1.318
d32 = −29.1 2.120
d15 = −5.95 –
[11.1803]
d22 = 3.07 –
[11.1803]
LiTaO3 d22 = 2 d31 = −1 d33 = −21 1.064 0.4– 5 [11.1802] –
[11.1802] [11.1802] [11.1802]
RbTiOAsO4 (RTA) d31 = 3.8 d32 = 2.3 d33 = 15.8 1.064 0.35– 5.3 [11.1804] 400 [11.1804]
RTiOPO4 (RTP) d31 = 4.1 d32 = 3.3 d33 = 17.1 1.064 0.35– 4.3 [11.1804] 600 [11.1804]
ZnGeP2 d36 = 75 d14 = 69 d25 = 69 10.6 0.74– 12 3
[11.1800] [11.1800]
Lasers and Coherent Light Sources 11.10 Generation of Coherent Mid-Infrared Radiation by Difference-Frequency Mixing 805

of polarization of the pump and signal beam and depend- implemented during crystal growth [11.1806–1808], is
ing on positive or negative birefringence of the crystal, becoming available.
the phase matching is called type I, type II or type III, as Equation (11.190)) is obtained under the assumption
defined in Table 11.50. For quasi-phase matching (see of infinite plane waves and no absorption. For Gaussian
below) all three beams have the same polarization. beams the relationship between idler power Pi , crys-
Equation (11.190) implies a possibility to generate tal length L, pump power Pp , signal power Ps , and
light at the idler frequency without phase matching. Ii absorption coefficient α is given by [11.1809–1811]:

Part C 11.10
has a maximum at ∆kL/2 = mπ/2, where m is a natu- 2 L
ral number. This yields the coherence length lc = π/∆k 32π 2 deff
Pi = Pp Ps h(ξ, σ, µ, α, L) .
after which the newly generated idler light will inter- ε0 cn i λi (n s λp + n p λs )
2

fere destructively with the light generated within the (11.192)


previous coherence length. Thus, after twice the coher-
The focusing function h(ξ, σ, µ, α, L) for diffraction-
ence length all generated light is destroyed. This can be
limited Gaussian beams is given by:
avoided by changing the polarization of the material by
180◦ after one or an odd multiple of the coherence length h (ξ, σ, α, L)
lc because this will change the sign of the nonlinear co- ⎛
efficient, so the light will interfere constructively and − αL
⎜e 2
a buildup of the generated light occurs, as illustrated in = Re ⎝

Fig. 11.200. This means that idler power can be gener-
ated without fulfilling the phase-matching condition by ⎞
ξ ξ −iσ(τ−τ )+ αL
4ξ (τ+τ )
using a periodically poled crystal. A quasi-phase match- e ⎟
× dτ dτ ⎠,
ing (QPM) condition can be written by using the grating 1 + ττ − i 1−µ
1+µ2

2 (τ − τ )
period Λ = 2lc of the crystal: −ξ −ξ
(11.193)
np ns ni 1
− − − =0. (11.191)
λp λs λi Λ where
For the same parameters as for the bulk material less L
ξ= , (11.194)
idler power will be generated for quasi-phase match- b
ing than for birefringent phase matching by a factor of
(2/π)2 . This factor is often included in deff by reduc- ks n s λp
µ= = , (11.195)
ing its value by a factor 2/π. Although the efficiency is kp n p λs
lower than in the case of birefringent phase matching,
more power can often be generated this way because  
np ns ni 1
the highest nonlinear coefficient can be used [e.g., σ = −πb − − − . (11.196)
λp λs λi Λ
for LiNbO3 d33 = −27 pm/V (Table 11.51) instead
of d22 = 3.07 pm/V, which is relevant for birefringent Here Λ is the grating period, and b is the confocal pa-
type II phase matching]. Since all involved polarizations rameter of both the pump and signal beam and is given
are the same (extraordinarily polarized, Table 11.50), by the minimal beam waist w : b = kp w2p = ks w2s , σ de-
the walk-off angle is zero, therefore longer crystals can scribes the phase mismatch. The focusing function h is
be used, resulting in higher idler power. Furthermore, discussed further below (see also Figs. 11.204, 205, 206
the selection of pump and signal wavelengths is rather and 11.208). These equations are valid for both bulk and
flexible. However, the production of periodically poled periodically poled crystals, only deff changes by a factor
crystals is difficult and not possible for all crystals. Un- 2/π compared to the case of a bulk crystal. The focusing
til now only LiNbO3 (PPLN), RbTiOAsO4 (PPRTA), function describes two competing effects: the efficiency
KTiOPO4 (PPKTP), and KTiOAsO4 (PPKTA) are is increased by focusing the beams because of higher in-
commercially available periodically poled. These are tensities, but at the same time reduced because of less
ferroelectric crystals that are poled by applying a strong collinear wavevectors. A possibility to overcome this
electrical field. Another, non-ferroelectric material is problem is to use waveguide periodically poled nonlin-
GaAs. In the beginning thin plates of GaAs with alternate ear crystals [11.1812]. Here the beams are confined in
polarization were stacked manually [11.1805]. Today a waveguide in the crystal leading to collinear wavevec-
orientation patterned GaAs, where the periodic poling is tors and high intensities at the same time. With this
806 Part C Coherent and Incoherent Light Sources

LiNbO3 [11.1817]:
IDFG
IDFG (4lc) n 2e = 5.35583 + 4.629 × 10−7 F
0.100473 + 3.862 × 10−2 F
+
λ2 − (0.20692 − 0.89 × 10−8 F)2
100 + 2.657 × 10−5 F
+ − 1.5334 × 10−2 λ2 .
λ2 − 11.349272
Part C 11.10

A (11.197)
Here F = (T − 24.5)(T + 570.82) describes the temper-
ature dependence when T is the temperature in ◦ C and
(2/ð)2 IDFG (4lc) λ is the wavelength in nm. This equation takes also
B the multiphonon absorption into account, which yields
more-accurate data for wavelengths between 4 µm and
5 µm.
When choosing the grating period and the tempera-
ture of the crystal, the thermal expansion of the crystal
C also needs to be taken into account because it also in-
0
lc lc z fluences the grating period, although much less than the
Polarization direction change of the refractive index with temperature. The
Nonlinear material
thermal expansion is (at 25 ◦ C) aa = 15 × 10−6 /◦ C and
ac = 7.5 × 10−6 /◦ C [11.1818] where the indices a and
Fig. 11.200 Idler power generation for phase-matching c correspond to the crystal axis. The refractive index of
condition ∆k = 0 (A), non-phase-matching condition LiNbO3 strongly depends on its composition, the Sell-
∆k  = 0 (C) and quasi-phase-matching condition in the case meier equation is for congruent composition, it will be
of a periodically poled crystal (B). lc denotes the coherence different for stoichiometric composition. Also the re-
length [11.1813] fractive index of MgO doped LiNbO3 , as often used in
experiments, differs from that of ordinary LiNbO3 .
technique continuous-wave (CW) idler powers in the
milliwatt range can be achieved whereas with bulk or pe- Nonlinear Crystals
riodically poled crystals the CW idler power is normally Numerous crystals show nonlinear optical effects, but
in the microwatt range. only a few are useful for difference-frequency gener-
The limit ξ → 0 gives the result for the infinite plane ation. The crystal material needs to be transparent at
wave because b → ∞ for plane waves. In this case the all wavelengths of pump, signal and idler beams, it
focusing function reduces to h ∼ ξ, resulting in an idler should have a high nonlinear coefficient and a high
power proportional to L 2 , as in the case for the plane damage threshold. In some cases, e.g., strong dispersion
waves (11.190). and weak birefringence, phase matching is not possible.
An often used nonlinear crystal for difference- These requirements limit the choice of nonlinear crys-
frequency generation in the mid-infrared is LiNbO3 tals. The optical properties of some nonlinear crystals
because it can be made periodically poled (known as used in DFG systems are listed in Table 11.51. Fig-
PPLN) and has a large nonlinear coefficient. Its effec- ure 11.201 shows the absolute nonlinear coefficient and
tive nonlinear coefficient is given by deff = 2/πd33 Mij = the transparency range of selected crystals for compari-
− 14.4 pm/V with d33 = −27 pm/V and Mij = 0.85 for son.
LiNbO3 at 3.3 µm [11.1814]. Mij is the Miller factor, For an easier comparison and characterization of
which describes the dispersion of the nonlinear coeffi- crystals and DFG setups reported in the literature the
cient [11.1800, 1815, 1816]. The factor 2/π is needed following figure of merit (FoM) is useful:
when using quasi-phase matching. Pi
To calculate the phase-matching condition the re- FoM = , (11.198)
fractive index needs to be known for all wavelengths. Pp Ps L
It is given by the temperature-dependent Sellmeier where Pi , Pp and Ps denote the power of the idler,
equation, e.g., for extraordinary polarized light in pump and signal beams, respectively, and L is the crystal
Lasers and Coherent Light Sources 11.10 Generation of Coherent Mid-Infrared Radiation by Difference-Frequency Mixing 807

AR coating often has a lower damage threshold than


Absolute nonlinear coefficient (pm/V) the crystal itself. At high power of the pump laser other
CdGeAs2 effects such as optical parametric generation (OPG) or
amplification (OPA) could become even stronger than
the difference-frequency generation, resulting in an en-
larged line width. If the signal laser has much more
100
power than the pump laser, pump depletion might be

Part C 11.10
ZnGeP2
GaSe
a problem. Therefore pump and signal laser and non-
linear crystal have to be carefully matched. To estimate
CdSe
AgGaSe2 how low the signal power needs to be to avoid pump
PPLN
HgGa2S4 depletion, the following formula can be used:
KNbO3 AgGaS2
PPRTA 2 L2 I
8π 2 deff
Ii s
PPKTA η= = 1, (11.199)
10 AgAsS3 Ip ε0 n p n s n i cλ2i
PPKTP
where Ii , Ip , and Is denote the idler, pump, and sig-
KTA
LiO3 LiNbO3 nal intensity, respectively, deff is the effective nonlinear
RTA
KTP coefficient, L is the crystal length, λi is the idler wave-
KDP length, ε0 is the dielectric constant and n is the refractive
index with the subscripts p, s, and i referring to pump,
signal and idler, respectively. η is the conversion effi-
1 CLBO ciency from pump beam to idler beam, where η = 1
LBO
implies that 100% of the pump beam is converted to
ADP the idler beam. This case gives the nonlinear interac-
BBO tion length L nl , one of several characteristic lengths of
SiO2
a DFG system

0.1 1 10
Transparency range (µm) ε0 n p n s n i cλ2i
L nl = 2 I
. (11.200)
8π 2 deff s
Fig. 11.201 Transparency range of some selected nonlinear
crystals used for mid-IR DFG generation as a function of Crystal lengths longer than L nl will not increase the idler
the absolute value of the nonlinear coefficient. For the peri- power because of pump depletion. The aperture length
odically poled materials (PPLN, PPRTA, PPKTA, PPKTP), L an is the distance after which the beam is displaced by
the nonlinear coefficient d33 is given [11.1813] 2w0 because of walk-off effects and is given by:
√ w0
L an = π , (11.201)
length. This way the comparison is independent of the ρn
laser powers and crystal lengths chosen. In Table 11.52
where w0 is the minimal beam waist and ρn is the walk-
this FoM is listed for some representative setups in-
off angle. The diffraction length L diff is the length after
volving various crystals and combinations of pump and
which
√ the beam diameter has increased by a factor of
signal lasers. Some of the setups generate a CW idler
2. Longer crystals will not increase the idler power.
beam by using two CW lasers for pump and signal; other
This effect can be calculated more precisely by using
setups have a pulsed idler beam by using two pulsed
the focusing function in (11.192).
lasers or one pulsed and one CW laser.
When choosing the pump and signal lasers several L diff = 4kw20 . (11.202)
issues have to be considered. The laser wavelengths need
to be within the transparency range of the crystal, and For pulsed lasers the interaction length L qs represents
the wavelengths and the polarizations should be chosen a further important issue
 
so that phase matching is possible. Another important √ 1 1 −1
aspect is the laser power. As the conversion efficiency is L qs = πτ − , (11.203)
vg1 vg2
rather low, high laser powers are preferred, but too-high
powers will damage the crystal, the surface of the crys- where τ is the pulse duration, vg1 and vg2 are the group
tal or the antireflection (AR) coating on the crystal. The velocities of the pump and the signal beams, respec-
808 Part C Coherent and Incoherent Light Sources

Table 11.52 Figure of merit (FoM) for different setups and crystals. PP: periodically poled, OP: orientation patterned, ECDL:
external-cavity diode laser
Crystal Pump laser Signal laser Idler Idler Figure of
wavelength power (µW) merit
(µm) (µW/(W2 cm))
LiNbO3 bulk ECDL 795–825 nm Nd:YAG 1064 nm 3.16–3.67 CW 0.030 0.4
Part C 11.10

[11.1819] 25–30 mW CW 1 Watt CW


PPLN [11.1820] ECDL 1030–1070 nm, Er-fiber laser 1545– 1605 nm 2.9–3.5 CW 3500 200
with Yb-fiber amplifier 5 W CW
700 mW CW
PPLN [11.1821] Nd:YAG 1064 nm ECDL 1500– 1600 nm 3.2–3.7 Pulsed 2000 4.4 × 105a
pulsed 6 ns rep. 4 –8 kHz 5 mW CW Average 4.4 × 105b
5 kW peak power power
PPLN [11.1814] ECDL 808 nm Nd:YAG 1064 nm 3.3 CW 27 410
20 mW CW 660 mW CW
PPLN [11.1809] Diode laser master/slave Nd:YAG 1064 nm 4.15–4.35 CW 172 110
848–855 nm with Yb-fiber amplifier
78 mW CW 5 W CW
PPLN ECDL 850–870 nm Nd:YAG 1064 nm 4.3–4.7 CW 5–23 4–19
This setup 125 mW CW 2 W CW
(see Sect. 11.10.3)
Waveguide PPLN Diode laser 940 nm ECDL 1550 nm 2.30–2.44 CW 400 1.2 × 105
[11.1812] 17.5 mW CW 20 mW CW
AgGaS2 [11.1822] ECDL 679–683 nm Diode laser 786– 791 nm 4.9–5.1 CW 0.1 31
40 mW CW 20 mW CW
AgGaSe2 [11.1823] Fabry-Perot diode laser ECDL 1504– 1589 nm 7.1–7.3 CW 0.010 52
1290 nm 6 mW CW
8 mW CW
PPKTP [11.1824] Nd:YAG 1064 nm ECDL 1490– 1568 nm 3.2–3.4 CW 0.170 22
222 mW CW with Er-fiber amplifier
34 mW CW
PPKTA [11.1825] Nd:YAG 1064 nm ECDL 1519 nm 3.45–3.75 CW 0.140 70
117.2 mW CW 17.4 mW CW
PPRTA [11.1826] Ti:Al2 O3 laser 710 –720 nm Ti:Al2 O3 laser 874–915 nm 3.4–4.5 CW 10 250
100 mW CW 200 mW CW
OP GaAs [11.1808] DFB diode laser ECDL 1535– 1570 nm 7.9 CW 0.038 6
1306–1314 nm with Er-fiber amplifier
1.5–3.3 mW CW 1 W CW
GaSe [11.1827] Nd:YAG 1064 nm OPA 1100–4800 nm 2.4–28 Pulsed 5 µJ 0.0041a
pulsed 20 ps pulsed 5 ps 2.1 × 106b
750 µJ rep. 10 Hz 35–50 µJ
LiInS2 [11.1828] Ti:Sapphire Ti:Sapphire 5.5–11.3 CW - 12.4
700–810 nm CW 800–900 nm CW
ZnGeP2 [11.1829] OPO signal 1760–1950 nm OPO idler 2710– 2330 nm 5 –12 Pulsed 25 µJ 0.2a
pulsed 7 ns, rep. 17 Hz pulsed 7 ns, rep. 17 Hz 1.6 × 106b
0.95 mJ 0.95 mJ
a FoM calculated with peak powers
b FoM calculated with average powers
Lasers and Coherent Light Sources 11.10 Generation of Coherent Mid-Infrared Radiation by Difference-Frequency Mixing 809

tively. L qs describes the length after which the pulses


Line strength (cm–1/molecule cm–2)
from the two beams are separated by τ. Another char-
400 × 10–21
acteristic length for pulsed laser is the dispersion length 300
L ds , given by 200 CO
100
τ2 0
L ds = , (11.204)
1 × 10–18
gn
0.8

Part C 11.10
where gn is the group-velocity dispersion. This length 0.6
0.4 N 2O
describes the length after which the pulse duration has 0.2
doubled. With these characteristic lengths first estima- 0
tions for crystal lengths and pulse durations can be 3 × 10–18
CO2
made. 2
1
11.10.2 DFG Laser Sources 0
2500 2100 2200 2300 2400 2500
Wavenumber (cm–1)
The literature on DFG laser sources, new nonlinear
crystal materials and applications has become exten- Fig. 11.202 Absorption lines of CO, N2 O and CO2 as
sive in recent years. By far the largest part of these a function of wavenumber in the mid-IR region [11.1830]
systems have been, and still are, developed for spectro-
scopic gas sensing and analysis application. A recent be neglected. The absorption coefficient at 4.3 µm is
overview of systems is given in reference [11.1813]. 0.25 cm−1 , at 4.6 µm it is 0.55 cm−1 and at 4.7 µm
In the following we describe a typical DFG setup that 0.75 cm−1 [11.1831]. There are other crystals that can
has been implemented in our laboratory for measure- be used at this wavelength, e.g., AgGaS2 or AgGaSe2
ments on isotopomers of trace gases. Precise isotope (Table 11.51), but they are not available periodically
ratio measurements of trace gases represent an impor- poled, so birefringent phase matching has to be used.
tant contribution to the solution of key questions in This means the crystal length needs to be shorter be-
various areas, e.g., differentiation between natural and cause of walk-off effects and it is not possible to use
anthropogenic origin of specific compounds. Isotopic the maximum nonlinear coefficient. Furthermore align-
compositions are of interest in such diverse fields as ment is more critical than with a periodically poled
ecological CO2 exchange, volcanic emission, medical crystal. Finally, wavelength tuning is also an important
diagnostics, extraterrestrial atmospheres, etc. issue. When working with such crystals angle tun-
ing has to be used, which makes wavelength tuning
Detailed Discussion of a DFG Laser Source over larger ranges more complicated. Often noncritical
Isotopic composition of trace gases such as CO2 , CO or phase matching is used, because of its larger accep-
N2 O are of special interest. These molecules with their tance bandwidth, but for a certain idler wavelength the
isotopomers exhibit strong absorption lines between 4.3 pair of signal and pump wavelength is fixed in this
to 4.7 µm (Fig. 11.202). Therefore a continuous-wave case. This limits the choice of lasers and normally two
DFG source, which enables continuous tuning and nar- diode lasers with lower power than other lasers have to
row line width (to differentiate between isotopomers), be used.
was implemented. In the following sections the theoret- In contrast, when using quasi-phase matching, the
ical calculations, the setup and the characterization of phase matching is realized by choosing a grating pe-
this system is described. riod, so nearly every combination of lasers can be
used (e.g., an external cavity diode laser (ECDL) that
Calculations of optimal crystal length and beam pa- can be conveniently wavelength tuned, and a Nd:YAG
rameter. For the wavelengths of interest we chose laser that delivers high laser power). Phase matching
LiNbO3 as nonlinear optical medium because it has is achieved by choosing the correct grating period Λ,
a transmission range from 0.4 µm to 5.0 µm, a large which can be adjusted to other wavelengths by changing
nonlinear coefficient, and it can be produced periodically the temperature of the crystal because of the tempera-
poled. ture dependence of the refractive index (11.197). When
However, LiNbO3 has an absorption band at 5 µm scanning the wavelength for spectroscopy, the crystal
so the absorption between 4 µm and 5 µm cannot temperature can be changed simultaneously to achieve
810 Part C Coherent and Incoherent Light Sources

1064 nm and a crystal length of 5 cm (Fig. 11.208), so


ëi the maximum idler power is not obtained at perfect phase
matching, but for a slightly different grating period.
However, to simplify the calculations, σ was set to 0. The
50 mm focusing function and hence the idler power has a clear
ë maximum at about ξ = 1.3 (Fig. 11.204). It depends only
0.5 mm
slightly on wavelength and absorption. Therefore for
6 mm
Part C 11.10

ëp a chosen crystal length L there is an optimal confocal


ës
parameter b.
Fig. 11.203 A periodically poled crystal with several grat- When the idler power is plotted as a function of crys-
ings for different wavelengths. λp,s,i : pump, signal, idler tal length L and of the confocal parameter b, it can be
wavelength, respectively; Λ: grating period seen that a long crystal combined with a large confo-
cal parameter yields higher idler power (Fig. 11.205).
mid-IR wavelength ranges of several hundred nm with However, in a real experiment the confocal parameter
only one grating period. Depending on wavelength the is limited by the thickness of the crystal and crystals
temperature acceptance bandwidth can be quite large longer than 6 cm are not easily commercially available.
(Fig. 11.209b). Even larger wavelength ranges can be The problem with longer crystals is that crystal defects
achieved by using a crystal with several gratings, as have too much influence. The thickness of the crystal
shown in Fig. 11.203. Typical grating periods for our is limited by the production process of the periodically
wavelength range are approximately 23 µm. As a result poled grating. This is done by applying an electric field
it appears advantageous to use PPLN for the envis- to change the orientation in the crystal, which requires
aged 4.3–4.7 µm wavelength range rather than a bulk very strong field strengths. This limits the thickness to
AgGaS2 or other crystal despite the non-negligible ab- 1 mm. Most crystals have a thickness of 0.5 mm, result-
sorption of PPLN. ing in a better grating quality than for a thickness of
According to (11.192) the idler power increases with 1 mm.
the crystal length but also the absorption increases, In Fig. 11.206 it can be seen how the idler power
therefore there is an optimum crystal length for this changes for different crystal lengths. The calculations
wavelength region. The maximum of the focusing func- were made with σ = 0 and keeping ξ = L/b = 1.3
tion h (11.193) is not at σ = 0 but, e.g., at σ = 1.3 for at the maximum. The result is that at λp = 853 nm
a pump wavelength of 863 nm, a signal wavelength of (λs = 1064 nm, λi = 4.3 µm) the optimal length is longer

h (î )
Pi (L, b) (µW)
50 × 10–3
350
40 300
250
30
200
20 150
100
10
9
0 8
7
0 2 4 6 8 10 6 8 9
5 7
î L (cm) 4 5 6
3 3 4
2 2 b (cm)
Fig. 11.204 Focusing function h(ξ) versus ξ calculated for
λp = 868 nm, λs = 1064 nm, α = 0.75 cm−1 , σ = 0, and Fig. 11.205 Idler power Pi versus crystal length L and con-
L = 5 cm. The maximum is at ξ = 1.3 and for small ξ the focal parameter b calculated at a pump wavelength of
focusing function h is proportional to ξ. The symbols are 853 nm. The idler power increases with increasing crystal
explained in (11.192, 193, 194, 195, 196) length and confocal parameter
Lasers and Coherent Light Sources 11.10 Generation of Coherent Mid-Infrared Radiation by Difference-Frequency Mixing 811

Idler power (µW) Idler power (µW) Idler power (µW)

200
80 50

150 40
60
30

Part C 11.10
100
40
20
50 20
ëp = 853 nm ëp = 863 nm 10 ëp = 868 nm

0 2 4 6 8 10 0 2 4 6 8 10 0 2 4 6 8 10
Crystal length (cm) Crystal length (cm) Crystal length (cm)

Fig. 11.206 Idler power as a function of crystal length for pump wavelengths λp of 853 nm, 863 nm, 868 nm. The signal
laser is a Nd:YAG laser fixed at λs = 1064 nm. The calculations were made with σ = 0 and keeping ξ = L/b = 1.3 at the
maximum. At 853 nm the ideal crystal length is longer than 10 cm, at 863 nm it is 5.9 cm, at 868 cm it is 4.0 cm

than 10 cm, at λp = 863 nm (λi = 4.6 µm) it is 5.9 cm, beam polarization for quasi-phase matching in the PPLN
and at λp = 868 nm (λi = 4.7 µm) it is 4.0 cm. We chose crystal. A small part of the pump beam is directed to
a crystal length of 5 cm, implying b = 4 cm, which a wavemeter. The recorded pump wavelength then yields
gives a minimal beam waist of 0.13 mm. Such a Gaus- the idler wavelength. After the crystal a germanium fil-
sian beam propagates within the crystal over the whole ter is used to block the near-infrared light. The setup is
length. depicted in Fig. 11.207.
Based on (11.192), an idler power of 55–170 µW is This DFG system was tested and characterized
expected for a pump power of 150 mW, a signal power by focusing the mid-IR beam onto a detector (VIGO
of 2 W and a crystal length of 5 cm. PDI-2TE-5, TE-cooled) and recording the signal with
a lock-in amplifier with a time constant of 100 ms.
Setup and characterization. Our DFG system con- For modulating the laser power with a frequency of
sists of an external cavity diode laser (EDCL) as pump 1.8 kHz, a chopper was placed after the Nd:YAG laser.
laser, a continuous-wave Nd:YAG laser as signal laser To find the crystal temperature for phase matching,
and a MgO-doped periodically poled LiNbO3 crystal the temperature was increased in steps of 0.2 ◦ C or
(MgO:PPLN). The ECDL (Sacher TEC-120-850-150) 0.5 ◦ C while keeping the pump wavelength constant
has a power of 150 mW and a wavelength range of (Fig. 11.208).
820–875 nm. To cover the idler wavelength range of The temperature for phase matching is 6.6–11.2%
4.3–4.7 µm, pump wavelengths of 852–868 nm are higher than theoretically calculated (Fig. 11.209a) and
needed. The Nd:YAG laser (Innolight Mephisto) has
a CW power of 2 W and a wavelength of 1064.5 nm.
The MgO:PPLN crystal (HC-Photonics) is 5 cm long ë/4 ë/2
plate plate
and 0.5 mm thick. It has several gratings with periods Nd:YAG Mirror
of 21.45, 22.00, 22.50, 23.10, and 23.65 µm, each with laser
Lens Lens Mirror
a width of 1.2 mm. For the wavelength of interest in Wavemeter
this experiment, only the grating period of 23.1 µm Mirror
is needed, it is quasi-phase matched for the different ë/2 Mirror
wavelengths by changing the temperature from 30 ◦ C to Ol plate Lens Filter
130 ◦ C. The crystal is antireflection coated for the pump, Diode Mid-IR
laser laser beam
signal and idler wavelengths. Lens PBS DBS PPLN Lens
The laser beams are focused by several lenses (in-
cluding cylindrical lenses, not shown in Fig. 11.207) so Fig. 11.207 Setup for difference-frequency generation. OI: optical
that the minimal beam radius is 0.13 mm within the isolator, PBS: polarizing beam splitter, DBS: dichroic beam splitter,
crystal. The λ/4 and λ/2 plates are used to match the PPLN: periodically poled LiNbO3
812 Part C Coherent and Incoherent Light Sources

Fig. 11.208 (a) Idler power as a func-


a) Idler power (µW) b) Idler power (µW) tion of phase mismatch σ (11.196),
200 ëp = 863,5 nm calculated for a pump wavelength
ëp = 863 nm 8 of 863 nm, a signal wavelength of
150 1064 nm, and a crystal length of 5 cm.
6
(b) Measured idler power as a function
100
4 of crystal temperature corresponding
Part C 11.10

50
to phase mismatch, at a wavelength of
2
863.5 nm and a crystal length of 5 cm.
0 0 It can be seen that the measured and
–10 –5 0 5 10 100 95 90 85 80
the calculated curve have a similar
Phase mismatch ó Crystal temperature (° C)
shape

the temperature acceptance bandwidth increase for conventional mass spectrometry but laser spectroscopy
longer wavelengths and is 2.5–3.7 ◦ C (Fig. 11.209b). enables an easy identification. Our measurements were
The power of the CW mid-infrared beam amounts to done with the DFG system described above and direct
23 µW at 4.3 µm and 5 µW at 4.76 µm (Fig. 11.209c). absorption spectroscopy with an astigmatic Herriot cell
It decreases for increasing wavelengths because of the (New Focus 5611) with an optical path length of 10 m.
crystal absorption near 5 µm. The generated idler power The setup is shown in Fig. 11.210.
is about four to ten times lower than calculated, most One problem in measuring isotopomers is that
probably because of imperfections in the crystal, its grat- the concentration of the main isotopomer is typically
ing quality and non-Gaussian beam shape of the ECDL a hundred times higher than that of the less-abundant
pump laser. isotopomer. There are two possibilities to overcome this
For measurements of the isotopic composition of problem, either to measure two lines of similar strength
trace gases, the laser line width should be sufficiently resulting in a strong temperature sensitivity of the mea-
narrow to resolve adjacent molecular lines clearly, also surement, or by choosing lines with similar lower energy
when recorded at reduced gas pressure. The line width levels but with very different line strength. The astig-
of our CW mid-IR source has been determined as ap- matic multipass Herriot cell offers the possibility to enter
proximately 1 MHz and thus fulfills the requirements by the cell at a different angle than usual, so that the beam
far. leaves the cell after only two passes (Fig. 11.210). This
makes it possible to measure two lines of very differ-
Measurement of isotopic composition of trace gases. ent line strength by using two different path lengths (the
We measured the isotopic ratios of 13 C/12 C and balanced-path-length detection scheme) [11.1832].
18 O/16 O in CO and CO, and of 15 N/14 N in N O. N O As an example, Fig. 11.211 shows the result of
2 2 2
is of special interest because 14 N15 N16 O and 15 N14 N16 O a measurement on CO2 isotopomers in ambient air at
have the same mass, so they cannot be distinguished by a concentration of 350 ppm. The measurements were

a) Temperature (° C) b) Acceptance bandwidth (° C) c) Idler power (µW)


120 Theory 3.6
Measurement 20
100 3.4
15
3.2
80
3.0 10
60
2.8
40 5
2.6
0
850 855 860 865 870 4.3 4.4 4.5 4.6 4.7 4.3 4.4 4.5 4.6 4.7
Wavelength ECDL (nm) Wavelength idler (µm) Wavelength (µm)
Fig. 11.209 (a) Quasi-phase-matching temperature as a function of pump wavelength. (b) Acceptance bandwidth as
a function of the temperature. (c) Idler power as a function of the idler wavelength
Lasers and Coherent Light Sources 11.10 Generation of Coherent Mid-Infrared Radiation by Difference-Frequency Mixing 813

Reference
11.10.3 Outlook
detector
Tunable coherent sources in the mid-infrared range
Multipass cell play an important role. This is manifested by the ever-
growing number of publications. The development is
fostered by numerous applications, primarily in gas
DFG
system sensing. The requirements with respect to sensitive and

Part C 11.10
Signal detector selective monitoring devices with multicomponent capa-
bility are manifold: access to a broad wavelength range,
Fig. 11.210 Setup for transmission spectroscopy. In the broad – preferentially continuous – wavelength tunabil-
astigmatic Herriot cell there are two paths, one of 10 m ity, narrow line width (i. e., much narrower than typical
(solid line) and one of 40 cm (dashed line) molecular absorption line widths), preferentially room-
temperature (RT) or near-RT operation, and compact
performed at a total pressure of 50 mbar and at room and robust setups for field applications. In this respect,
temperature. The experimental data are fitted with DFG systems represent a very valuable choice. Since
Voigt curves to calculate the concentrations of the iso- their first realization in 1974 [11.1835], DFG-based
topomers. devices have reached a mature level. Today, their wave-
The derived isotope ratios of 13 C/12 C for CO2 length range can be chosen between, e.g., 2 µm and
are 1.3% ± 0.2% (only long path) and 1.4% ± 0.3% 19 µm only depending on the available pump and sig-
(balanced-path-length detection scheme), which is in nal sources and nonlinear crystals. The tuning of a DFG
good agreement with the natural abundance of 1.1%. source is straightforward and continuous, and the wave-
The isotope ratio 18 O/16 O of CO2 is deduced as length generated can be accurately determined via the
0.44% ± 0.06% (only long path) and 0.47% ± 0.11% near-infrared input wavelengths. The line width is ba-
(balanced-path-length detection scheme), which again sically given by the line width of the pump and signal
is in good agreement with the natural abundance of laser. This enables narrow mid-IR line widths as re-
0.39%. A more-detailed discussion of these studies, quired for high-resolution spectroscopy. In contrast to
which also includes measurements of CO and N2 O iso- alternative mid-IR sources, DFG systems are generally
topomers, can be found in [11.1833]. A further study on room-temperature devices except for the crystal, which
N2 O isotopomers, testing different detection schemes may require heating in a small temperature-controlled
for low concentrations (100 ppm) has been published oven. Line widths of continuous-wave DFG sources
in [11.1834]. are in the MHz range, which makes them attractive

Res. × 10–6 Res. × 10–6


20 200
0 0
–20 –200

Absorption coefficient (cm–1) Absorption coefficient (cm–1)


13 –3
300 × 10
–6 CO2 2 × 10
12 16
C O2
250
18 12 16 1.5
200 O C O

150 1
100
0.5
50
0 0
2309.2 2309.25 2309.3 2309.35 2309.4 2308.54 2308.56 2308.58 2308.60 2308.62
–1
Wavenumber (cm ) Wavenumber (cm–1)
Fig. 11.211 Absorption lines of different isotopomers of 350 ppm CO2 in ambient air. Experimental data (dots) and Voigt
fit (solid line) for 10 m path length, residuals on top
814 Part C Coherent and Incoherent Light Sources

for studies requiring high spectral resolution such as rent developments in several areas appear promising:
the briefly discussed isotopomer measurements. DFG the availability of compact and powerful signal and
sources are rather low-power lasers with CW powers pump lasers, fiber amplifiers, new nonlinear crystal
in the µW to mW range. With fiber amplifiers for the materials including organic media to access further
near-IR pump and signal sources, higher powers can be wavelength ranges, new materials with higher non-
achieved if necessary [11.1820]. Recent developments linear optical coefficients, birefringent bulk crystals
in waveguide technology in PPLN [11.1812] or KTP with better quality, larger crystal sizes and higher
Part C 11.11

appear particularly attractive in view of higher conver- damage thresholds, quasi-phase matching becoming
sion efficiencies. Last but not least, a DFG system can available for more crystals than today, waveguide
be made compact in view of today’s diode lasers and technology, etc. These developments will contribute
diode-pumped solid-state lasers used as pump and signal to improve the performance of DFG devices, en-
sources. hance their distribution, lower their costs and hence
In view of the variety of applications a further further increase their role as attractive spectroscopic
impetus for DFG systems can be expected. Cur- tools.

11.11 Free-Electron Lasers


The free-electron laser (FEL) is a system consisting of The scale of the FEL setup is mainly defined by the scale
a relativistic electron beam and a radiation field inter- of the driving accelerator. For FELs operating in the mil-
acting with each other while they propagate through limeter wavelength range this could be a room scale,
an undulator [11.1836, 1837]. The main components while unique devices such as VUV and X-ray FELs
of the free-electron laser are electron accelerator, un- user facilities have a scale comparable with conven-
dulator, and optical resonator (optionally for an FEL tional third-generation synchrotron radiation facilities
oscillator). The undulator is a periodic magnetic struc- (Fig. 11.212).
ture with a planar, or helical magnetic field that causes
periodical transverse deflections of the electron-beam 11.11.1 Principle of Operation
trajectory [11.1838]. Optical resonators are fairly sim-
ilar to those used in conventional lasers. FEL devices The FEL is not actually a laser; it is most closely re-
have been realized with nearly all types of accelera- lated to vacuum-tube devices. As with vacuum-tube
tors: electrostatic accelerators, RF linear accelerators, devices, FEL devices can be divided in two classes:
induction accelerators, microtrons, storage rings, etc. amplifiers and oscillators (Fig. 11.213). An FEL ampli-
The wavelength range covered by FELs spans from cen- fier is a single-pass device, and there is no feedback
timeters down to nanometers [11.1839] (Table 11.53). between the output and input. The FEL oscillator can
be considered as an FEL amplifier with feedback. For
Table 11.53 Parameter space of free-electron lasers as of
an FEL oscillator in the optical wavelength range the
2006 feedback is carried out by means of an optical resonator.
Radiation FELs based on the oscillator principle are limited on the
Wavelength 13 nm–10 mm short-wavelength side to ultraviolet wavelengths primar-
Peak power up to 5 GW ily because of mirror limitations. Free-electron lasing at
Average power up to 10 kW wavelengths shorter than the ultraviolet can be achieved
Pulse duration 10 fs to CW with a single-pass high-gain FEL amplifier.
Driving electron beam The field of the electromagnetic wave only has trans-
Energy 200 keV–1 GeV verse components, so the energy exchange between the
Peak current 1–3000 A
electron and the electromagnetic wave is due to the
transverse component of the electron velocity. The lat-
Undulator
ter occurs due to periodical wiggling of the electron in
Period 0.5–20 cm
the undulator. The driving mechanism of free-electron
Peak magnetic field 0.1–1 T
lasers is the radiative instability of the electron beam,
Undulator length 0.5–27 m which develops due to the collective interaction of elec-
Lasers and Coherent Light Sources 11.11 Free-Electron Lasers 815

trons with the electromagnetic field in the undulator.


The basic principle of radiation-induced instability can
be described within the standard picture for the gener-
ation of the synchrotron radiation. Electrons propagate
along a sinusoidal path and emit synchrotron radiation
in a narrow cone in the forward direction. When an
electron beam traverses an undulator, it emits radiation

Part C 11.11
at the resonance wavelength λ = (λw /2γ 2 )(1 + K 2 /2).
Here, λw is the undulator period, mc2 γ is the electron
beam energy, K = eHw λw /2πmc is the dimensionless
undulator strength parameter, and Hw is the maximum
on-axis magnetic field strength of the undulator. Al-
though the electromagnetic wave is always faster than
the electrons, a resonant condition occurs such that the
radiation slips a distance λ relative to the electrons af-
ter one undulator period. The fields produced by the
moving charges in one part of the undulator react on
moving charges in another part of the undulator. Thus,
we deal with some tail–head instability, which leads to
a growing concentration of particles wherever a small
perturbation started to occur (Fig. 11.214). In the begin-
ning – without microbunching – all N electrons can be
treated as individually radiating charges producing the
power of the spontaneous emission ∝ N. With complete
microbunching, all electrons radiate almost in phase. Fig. 11.212 Aerial view of the experimental hall for the FLASH user
This leads to a radiation power ∝ N 2 and thus to an am- facility in Hamburg (center) and the tunnel for the superconducting
plification of many orders of magnitude with respect to accelerator and undulator (covered with grass). The hall in the up-
the spontaneous emission of the undulator. per right corner houses the injector part of the linac. The total length
The figure of merit for FEL performance is the ra- of the FLASH facility is 300 m. The maximum energy of electrons
diation power gain during one pass of the undulator. is 1 GeV, and the minimum radiation wavelength is 6 nm. The undu-
The gain primarily depends on the value of the peak lator of the FLASH (photo in the upper left corner) is a permanent
beam current. Another quantity of importance for the magnet device (period 2.73 cm, gap 12 mm, peak field 0.47 T). The
development of the radiative instability is the electron undulator system is subdivided into six segments, each 4.5 m long
beam density in the six-dimensional phase space. Low
beam quality (large energy spread and emittance) leads
to degradation of the FEL gain. Errors in the periodi- degree of transverse coherence. In other words, the FEL
cal magnetic structure also degrade FEL performance. radiation can always be focused on to a spot whose size
Presently accelerator techniques and undulator technol- is defined totally by diffraction effects. This feature re-
ogy have reached such a level that it is possible to have veals a wide range of possibilities for FEL applications
power gains of the order of 107 for the amplification of in the transportation of the radiation over long distances
the radiation of a nanometer wavelength range. and in obtaining high focused intensities.
However, FELs are relatively expensive devices,
11.11.2 Current Status and Perspective thus their applications are in the fields not covered
Applications of Free-Electron Lasers by conventional radiation sources, in the far-infrared
wavelength range and the THz gap (the sub-millimeter
Free-electron lasers hold several potential advantages: wavelength range). Another field for FEL applications
continuous tunability of the radiation wavelength, the is the generation of short-wavelength radiation, from the
possibility to obtain high levels of average output power, vacuum ultraviolet down to X-ray range. Technological
and the possibility to obtain high conversion efficiencies developments are on the way, aiming at industrial appli-
of the net electrical power to radiation power. An im- cations of powerful FELs, and the use of FELs for energy
portant feature of the FEL radiation is that it has a high transfer in space is also under consideration. Organiza-
816 Part C Coherent and Incoherent Light Sources

power in the MW range, and micropulse repetition rate


Mirror Undulator Output in the range 10 MHz to 3 GHz. FELs driven by nor-
radiation
mal conducting RF accelerators operate in pulsed mode
with a macropulse repetition rate of 10–100 Hz. The
macropulse duration is defined by the length of the RF
pulse, typically 1–20 µs. Thus, the average radiation
Electron beam
power is in the watt range. FELs driven by superconduct-
Part C 11.11

Undulator ing accelerators operate in continuous mode and produce


Seed radiation Output radiation a high level of average output power, up to a few kW.
Linac-based FEL facilities are recognized nowadays as
a unique tool for scientific applications that require tun-
able coherent radiation in the infrared wavelength range.
Electron beam The general tendency is that the wavelength region of
interest for users at these facilities is moving into the
Undulator
Output radiation far-infrared and THz gap.

FEL User Facilities at Storage Rings


Several storage rings are equipped with free-electron
lasers [11.1854–1857]. Typical parameters of the ra-
Electron beam
diation are: wavelength range of 190–700 nm, pulse
Fig. 11.213 Free-electron laser configurations: oscillator duration of some tens of picoseconds, average power
(top), seeded amplifier (middle), and self-amplified sponta- of 10–300 mW, and peak power in the kW range. Op-
neous emission (SASE) FEL (bottom) eration in a locked-mode regime allows the peak power
to be increased by an order of magnitude. The general
tion of user operation at the FEL facilities is similar to tendency is that users’ interest in these facilities is grad-
that used at synchrotron radiation facilities: the host or- ually reducing due to the limited features compared with
ganization constructs and serves free-electron laser and conventional lasers.
user beam lines, and users perform their experiments
according to the schedule of the facility. High-Average-Power FELs
Recent progress in accelerator technology has paved
Linac-Based FEL User Facilities the way for construction of high-average-power linear
There are several operating linear accelerator (linac)- accelerators. The quality of electron beams produced
based FEL user facilities (in China, France, Germany, by such machines are sufficient to drive free-electron
Japan, Korea, The Netherlands, Russia, and USA) work- lasers. Application of the energy-recovery technique al-
ing for scientific applications [11.1840–1853]. The lows a high level of overall efficiency to be achieved.
wavelength range covered with these facilities spans Pilot facility are already in operation in Japan, Rus-
from 200 nm to a few hundred micrometers. Typical sia, and USA [11.1851–1853]. The demonstrated level
parameters of the FELs driven by RF linear acceler- of the average radiation power is about 10 kW in the
ators are: pulse duration of a few picoseconds, peak 3–20 µm wavelength range [11.1852], and about 0.4 kW

–2 –1 0 1 2 –2 –1 0 1 2 –2 –1 0 1 2
z/ë z/ë z/ë

Fig. 11.214 Distribution of the electrons in the electron beam (longitudinal cut). The left, middle, and right snapshots are
taken at the beginning, middle, and the end of the undulator. Electron beam density is modulated periodically with the
period of the resonance wavelength due to the radiative instability
Lasers and Coherent Light Sources 11.11 Free-Electron Lasers 817

in the THz gap [11.1851]. Projects of next-generation A new era of synchrotron radiation research has
FELs based on energy-recovery linacs aim at increas- begun withthe first user experiments on a vacuum
ing the average power into the tens of kilowatt range, UV FEL based on self-amplified spontaneous emis-
and also to build high-power FELs operating in the UV sion (SASE) [11.1865, 1867]. It is worth mentioning
range [11.1858–1863]. that such an essentially quantum terminology [intro-
Potential industrial applications of high-average- duced after amplified spontaneous emission (ASE)]
power FELs involve material processing (for instance, does not reflect the actual physics of the process. The

Part C 11.11
the treatment of polymer surfaces), lithography, iso- amplification process in the SASE FEL has its ori-
tope separation, and chemical applications. Production gin in density fluctuations in the electron beam. The
of pure isotopes on an industrial scale may have a big latter effect is completely classical. The results have
impact on future developments. For instance, isotope been obtained at the TESLA test facility (TTF) at
28 Si is a radiation-resistant material of great interest the Deutsches Elektronen-Synchrotron DESY (Ham-
for space research and the nuclear energy industry. The burg, Germany), using radiation pulses at a wavelength
thermal conductivity of the pure isotope 28 Si is 50% of 98 nm with a 40 fs pulse duration and a peak
higher than that in the natural mixture, which seems power of 1.5 GW [11.1864, 1868] (Fig. 11.215). Com-
very attractive for the semiconductor industry. The are pared to present-day synchrotron radiation sources its
also many other isotopes of great practical interest such peak brilliance is more than 100 million times higher
as 13 C (medical applications) and 15 N (for the study (Fig. 11.216), the radiation has a high degree of trans-
and current control of use of nitrogen fertilizers in verse coherence and the pulse duration is reduced from
agriculture and agrochemistry). The basic process of hundreds of picoseconds down to ten-femtosecond time
isotope separation is a selective multiphoton dissocia- domain. While modern third-generation synchrotron
tion of molecules. The required resonance wavelength light sources are reaching their fundamental perfor-
range is in the range 2–50 µm. The required energy in mance limit, recent success in the development of the
a pulse is no less than 0.1 mJ and monochromaticity of VUV FEL at DESY has paved the way for the construc-
10−2 –10−4 , depending on the type of reaction. Indus- tion of a novel type of light source that will combine most
trial production of isotopes requires FELs with average of the positive aspects of both a laser and a synchrotron.
power exceeding 10 kW. Construction of such facilities In an X-ray FEL the radiation is produced by the
is on the way, and the first results are expected in the electron beam during a single pass of the undula-
near future. tor [11.1869–1871]. The amplification process starts
from shot noise in the electron beam. Any random fluc-
X-ray Free-Electron Lasers tuations in the beam current correspond to an intensity
At the start of this century, we have seen a revolu- modulation of the beam current at all frequencies simul-
tion in synchrotron source intensities. This revolution taneously – including of course, the frequency to which
stemmed from the technique of free-0electron lasers the undulator is tuned. When the electron beam enters
combined with recent progress in accelerator technolo- the undulator, the presence of the beam modulation at
gies, developed in connection with high-energy linear frequencies close to the resonance frequency initiates
colliders [11.1866]. X-ray FELS (XFELs) have made the process of radiation. The FEL collective instability
a new regime of intensities accessible, thus opening up in the electron beam produces an exponential growth
a fundamentally new physical domain. (along the undulator) of the modulation of the electron

Fig. 11.215 Left: Average energy


E (J)
10–4 in the radiation pulse versus un-
–5
dulator length for TTF FEL at
10
DESY [11.1864]. Right: interac-
10–6 tion of powerful VUV radiation with
10–7
solids [11.1865]. Ablation of a gold
target after one pulse of the TTF FEL
10–8 at DESY. The radiation wavelength
20 µm is 98 nm, the pulse duration is 40 fs,
10–9
0 2 4 6 8 10 12 14
z (m) and the peak power density is about
100 TW/cm2
818 Part C Coherent and Incoherent Light Sources

which the power increases by the factor of e = 2.718).


Peak brilliance (Photons/s mrad2 mm2 0.1% BW)
The spectrum of transversely coherent fraction of
1035
the radiation is concentrated within the narrow band,
XFEL ∆λ/λ  (2π Nw )−1 . The typical amplification band-
1033 width of the XFEL is of the order of 0.1%. The electron
FLASH
(seeded) LCLS
beam in an XFEL transfers enormous peak power. For
31
instance, for typical XFEL parameters (electron energy
10
Part C 11.11

of 17.5 GeV and peak current 5 kA) it is about 100 TW.


FLASH The conversion efficiency of kinetic energy of electrons
10 29 to the light is of the order of the amplification band-
width, thus the peak power of X-ray radiation is in the
multi-GW range (Table 11.54).
1027 Experimental realization of XFELs has developed
very rapidly during the last decade. The first demon-
1025 stration of the SASE FEL mechanism took place in
PETRA III 20m ID SPring-8
U29 1997 in the infrared wavelength range [11.1874]. In
UE65
ESRF
ID23
September 2000, a group at Argonne National Labora-
1023 tory (ANL) became the first to demonstrate saturation in
APS
U-A
BESSY a visible (390 nm) SASE FEL [11.1875]. In September
U-49
10 21 BESSY 2001, a group at DESY (Hamburg, Germany) demon-
U-125 PETRA II
ALS strated lasing to saturation at 98 nm [11.1864, 1868].
U5.0
In June 2006 saturation was achieved at 13 nm, the
1019 shortest wavelength ever generated by FELs. The
101 102 103 104 105 106
Energy (eV)
experimental results have been achieved at FLASH
(Free-Electron-LASer in Hamburg, Fig. 11.212). Regu-
Fig. 11.216 Peak brilliance of X-ray FELs versus third- lar user operation of FLASH started in 2005 [11.1872].
generation storage rings light sources. Circles show the Currently FLASH produces GW-level, laser-like VUV
experimental performance of the FLASH free-electron laser radiation pulses with 10–50 fs duration in the wave-
at DESY length range 13–45 nm. After the energy upgrade of
the FLASH linac to 1 GeV planned in 2007, it will be
density on the scale of undulator radiation wavelength possible to generate wavelengths down to 6 nm.
(Figs. 11.214, 215). The fluctuations of current density in Recently the German government, encouraged by
the electron beam are uncorrelated, not only in time but these results, approved funding of a hard-X-ray SASE
also in space. Thus, a large number of transverse radia-
tion modes are excited when the electron beam enters the Table 11.54 Main parameters of present and future X-ray
undulator. These radiation modes have different gains. FELs [11.1872, 1873]
Obviously, as undulator length progresses, the high-gain 2006: 2013:
modes will predominate increasingly and we can regard FLASH European XFEL
the XFEL as a filter, in the sense that it filters from ar-
Radiation
bitrary radiation field those components corresponding
Wavelength 13– 180 nm down to 0.1 nm
to the high-gain modes. Hence, for a long enough un-
Peak power up to 5 GW up to 150 GW
dulator, the emission will emerge in nearly complete
Average power 10 mW up to 500 W
transverse coherence. An intensity gain in excess of 107
Pulse duration 10–50 fs 0.2–100 fs
is obtained in the saturation regime. At this level, the
Driving electron beam
shot noise of the electron beam is amplified up to com-
Energy 0.3–0.7 GeV up to 20 GeV
plete microbunching, and all electrons radiate almost in
Peak current 1–3 kA up to 5 kA
phase, producing powerful, coherent radiation.
Undulator
The amplification bandwidth of a high-gain FEL
amplifier is restricted by the resonance properties of Period 2.73 cm 3.6–8 cm
the undulator, that is, by the number of undulator pe- Peak magnetic field 0.5 T 0.5–1.4 T
riods Nw within one gain length (the distance over Undulator length 27 m up to 200 m
Lasers and Coherent Light Sources 11.12 X-ray and EUV Sources 819

FEL user facility – the European X-ray free-electron 2. C. A. Brau: Free-Electron Lasers (Academic,
laser [11.1873]. The US department of energy (DOE) Boston 1990)
has given SLAC the go ahead for the engineering design 3. P. Luchini and H. Motz: Undulators and Free-
of the linac coherent light source (LCLS) device to be Electron Lasers (Clarendon, Oxford 1990)
constructed at SLAC [11.1876]. These devices should 4. W. B. Colson, C. Pellegrini and A. Renieri (Eds.):
produce 100 fs X-ray pulses with over 10 GW of peak Free Electron Lasers, Laser Handbook, Vol. 6 (North
power. New X-ray sources will be able to produce inten- Holland, Amsterdam 1990)

Part C 11.12
sities of the order of 1018 W/cm2 . The main difference 5. G. Dattoli, A. Renieri, A. Torre: Lectures on the Free
between these projects is the linear accelerator: an ex- Electron Laser Theory and Related Topics (World
isting room-temperature linac for LCLS at SLAC, and Scientific, Singapore 1993)
a future superconducting linac for the European XFEL. 6. H. P. Freund, T. M. Antonsen: Principles of
The XFEL based on superconducting accelerator tech- Free Electron Lasers (Chapman Hall, New York
nology will enable not only a jump in peak brilliance 1996)
of ten orders of magnitude, but also an increase by 7. E. L. Saldin, E. A. Schneidmiller, M. V. Yurkov: The
five orders of magnitude in the average brilliance. The Physics of Free Electron Lasers (Springer, Berlin,
LCLS and European XFEL projects are scheduled to Heidelberg 1999)
start operation in 2009 and 2013, respectively.
FEL Conference Proceedings
11.11.3 Suggested further reading In the period from 1985 to 2002 the FEL Conference
Proceedings have been published in Nuclear Instruments
Books and Methods, Section A. Starting from 2004 they are
1. T. C. Marshall: Free-Electron Lasers (Macmillan, collected in electronic form on a WEB page dedicated
New York 1985) to accelerator physics http://www.JACoW.org.

11.12 X-ray and EUV Sources


The extension of lasing into the X-ray region has been 11.12.1 X-Ray Lasers
investigated by a wide variety of methods since the
first demonstration of the visible laser in 1960. Al- The development of an X-ray laser has been one
though laser operation in the hard-X-ray region, which of the elusive dreams of laser physicists. Proposals
can be categorized as wavelengths shorter than 0.2 nm, for excitation schemes for X-ray lasers date back to
has not been realized, much progress on the develop- 1965, when the possibility of achieving soft-X-ray
ment of coherent light sources has been made in the amplification by collisional recombination was first sug-
soft-X-ray (0.2–30 nm) and extreme-ultraviolet (EUV, gested by Gudzenko and Shelepin [11.1877]. This was
30–100 nm) regions during these 20 years. There are two followed by proposals for photoionization pumping
major methods to produce coherent short-wavelength of X-ray lasers in 1967 [11.1878] and of electron-
radiation in these spectral regions. One is the use of impact excitation schemes [11.1879]. The latter were
transitions in highly charged ions in high-density plas- inspired in part by the earlier success in the devel-
mas created by laser irradiation of various targets or opment of visible and ultraviolet ion lasers excited
electric discharge. The other is the generation of very by electron collisions. However, the drastic scaling of
high harmonics of intense laser pulses. Each method the pump power requirements with decreasing wave-
has its advantages. X-ray lasers based on high-density length and the low reflectivity of optics at soft-X-ray
plasmas can produce much higher energy per pulse and wavelengths, combined with the short lifetime of the
narrower spectra. High harmonics can be generated with excited levels involved in the lasing process, made
compact, high-repetition rated lasers and produce a wide the realization of soft-X-ray lasers a very challeng-
range of the spectrum from 100 nm to 3 nm. The use of ing task [11.1880, 1881]. Several experiments carried
these sources depends on the application and will be out during the 1970s and early 1980s yielded the ob-
complementary. servation of population inversion and gain [11.1882].
820 Part C Coherent and Incoherent Light Sources

and were operated at a low repetition rate. Since sat-


Thin foil
urated amplification at a water window wavelength has
Optical laser light
not been accomplished even with the world largest
–2
10 cm laser driver [11.1891], a new excitation scheme has
–5
10 cm been sought for obtaining soft-X-ray lasers operating
at shorter wavelengths. Many efforts have been di-
Plasma rected in order to reduce the driver laser energy. The
Part C 11.12

reduction of the pump laser energy is essential for the


1 cm
X-ray laser light realization of tabletop X-ray lasers for potential appli-
cations [11.1892].
Fig. 11.217 Schematic drawing of an exploding-foil-target
X-ray laser Electron Collision Excitation
Ions with specific numbers of electrons have a fully
Nevertheless, the experimental demonstration of large occupied outer-shell structure and survive over a wide
amplification at soft-X-ray wavelengths was not realized range of plasma parameters. This is a significant ad-
until 1984. Matthews et al. [11.1883] at the Lawrence vantage for plasma X-ray lasers because it results in
Livermore National Laboratory reported soft-X-ray am- a high relative abundance of the lasing ions over a wide
plification at wavelengths of 20.6 and 21.0 nm in Ne-like range of temperature and density. To date, amplifica-
Se by electron collisional excitation. An exploding- tion has been observed in those ions. For example, the
foil-target X-ray laser demonstrated by Matthews et al. electronic structure of highly ionized selenium with 24
and the observed spectra are shown in Figs. 11.217 electrons removed (Se24+ ) is similar to that of neutral
and 11.218, respectively. In parallel with this, Suck- neon (Ne-like), and the transitions are also similar to
ewer et al. [11.1884] at Princeton University reported those of neutral neon [11.1893]. Such a comparison is
amplification at 18.2 nm in H-like C by recombination referred to as isoelectronic scaling of energy levels and
excitation. These pioneering works were soon followed transitions.
by numerous successful soft-X-ray amplification exper- Figure 11.219 shows a simplified energy-level di-
iments conducted using of the world’s most powerful agram of a Ne-like ion scheme. The 3p laser upper
lasers as pump sources [11.1885–1887]. Subsequent ex- states are populated mainly by electron collision ex-
periments achieved soft-X-ray laser operation in the citation from the 2p6 Ne-like ion ground state. The
saturated-gain regime [11.1888], and brought several population inversions are maintained by the rapid ra-
potential applications to fruition [11.1889, 1890]. These diative decay of the 3s lower states to the ground
applications include microscopy, holography, diagnos- state. The Ne-like scheme is well studied and is the
tics of dense plasmas, and the excitation of nonlinear most robust for electron collisional soft-X-ray lasers.
photoluminescence in crystals. In spite of their pio- However, it has the disadvantages that a large pump
neering works, these soft-X-ray lasers have not been power is required to produce population inversion at
used as a laboratory tool because both schemes re- a given wavelength. The nickel-like scheme was first
quired huge laser energies of several hundred joules proposed by Maxon et al. [11.1894] and proved to
be useful for shorter-wavelength amplification, below
10 nm [11.1895]. Although the lasing scheme of the Ni-
Off axis (a) like ions is directly analogous to that of Ne-like ions,
500
300 its higher quantum efficiency for a given ionization state
100
allows the required pumping energy to be significantly
reduced. Recently, gain-saturated amplification in the
300 Ni-like scheme has been obtained at wavelengths as
On axis (n)
200 short as 7.3 nm [11.1896].
100
0 Transient Collision Excitation
140 150 160 170 180 190 200 210 220 230 240 The transient collisional excitation (TCE) scheme first
Wavelength (Å)
proposed by Afanasiev and Shlyaptsev [11.1897] is
Fig. 11.218a,b Grazing-incidence spectrograph data from (a) off a variation of the electron collisional excitation. TCE
axis and (b) on axis has attractive properties such as:
Lasers and Coherent Light Sources 11.12 X-ray and EUV Sources 821

1. the gain coefficients are 1–2 orders of magnitude


2p5 3d
larger than those obtained for the same transition in 1 5
the quasi-steady-state regime, 2, 2 3

2. the required laser energy for amplification can be re- 3 5


2, 2 3
duced greatly, resulting in the realization of tabletop
X-ray lasers.
2p5 3p

Part C 11.12
In the TCE scheme, an intense picosecond laser pulse 1 1
2, 2 0
overheats the preformed plasma at a rate faster than other
collisional processes. The preformed plasma, containing Lasing transitions
1 3
2, 2 2
the lasing ions such as Ne-like and Ni-like ions, is pro- ë = 183Å
3 3
duced by a preceeding low-intensity nanosecond laser 209Å 2, 2 2
206Å
pulse. Transient gains in excess of 100 cm−1 have been
predicted theoretically. Similar to the quasi-steady-state 2p5 3s
scheme, the TEC was firstly demonstrated in an Ne-like 1 1
2, 2 1
ion [11.1898] and has been successfully applied to Ni-
3 1
like ions [11.1899]. Saturated amplification with a gain 2, 2 1
coefficient as high as 63 cm−1 has been reported from
Ni-like Pd at 14.7 nm with a total pump energy as low as
7 J [11.1900]. Figure 11.220 shows the evolution of the
14.7 nm laser line along the plasma column. Recently, 2s2 2p6 (0, 0)0
this scheme has been extended to lasing at 8.8 nm in
Ni-like La [11.1901]. Fig. 11.219 Simplified energy-level diagram for Ne-like Se

Optical-Field Ionization X-Ray Lasers of a quasistatic model, Burnett and Corkum [11.1904]
There are two kinds of plasma production scheme showed that cold dense multiply ionized plasmas could
for X-ray laser media by use of high-power lasers. be produced by OFI, which are suitable for recombina-
The optical-field ionization (OFI) scheme is completely tion X-ray lasers. Nagata et al. [11.1905] demonstrated
different from the conventional plasma production amplification of the Lyman α(n = 2 − 1) transition at
scheme. The OFI is direct ionization by a strong 13.5 nm in H-like Li by the recombination pumping
optical field, which modifies the Coulomb potential scheme following the OFI. Using a sub-picosecond KrF
of the atoms or ions to create electrons by tunnel-
ing ionization [11.1902]. In contrast to conventional
XRL intensity (arb. units)
X-ray laser schemes using electron collisional ioniza-
tion, the OFI scheme requires an intense laser power Ni-like Pd
103
rather than the large laser energy. Recent advances in 4d®4p
the technology of ultrashort-pulse generation and am- J=0®1
147 Å
plification have achieved laser powers high enough 102
to realize OFI X-ray lasers with a tabletop device.
The requirement for low pump energy will also al-
101
low soft-X-ray lasers to operate at high repetition
rates, which is critical for most of the promising
applications. 100
By applying this scheme to low-atomic-number me-
dia, a plasma consisting of fully stripped ions and free
electrons is produced on a time scale much shorter than 10–1
their collisional and radiative time. In other words, the
0 0.2 0.4 0.6 0.8 1
temperature of electrons produced by the OFI is not Length (cm)
determined by the charge state of ions, but can be con-
trolled separately by ionizing-laser parameters such as Fig. 11.220 Intensity of 14.7 nm X-ray laser line for
the polarization and wavelength [11.1903]. By means 1–8 mm Pd target lengths
822 Part C Coherent and Incoherent Light Sources

urated amplification of the 41.8 nm line in Pd-like Xe


Rotating target: Li
Filter with 0.6 J, 30 fs Ti:sapphire laser pulses. 5 × 109 photons
per pulse were obtained at gain saturation [11.1910].
0.5 mm XUV They also reported the lasing at 32 nm in nickel-like
Sub-picosecond spectrograph
On axis krypton [11.1911]. The experimental setup is shown
KrF laser
Off axis
(10 mrad) in Fig. 11.222.
Achromatic lens Slit
Part C 11.12

f = 300 mm Multichannel Discharge Excitation


f = 400 mm detector
Direct excitation of plasma X-ray lasers by an electrical
Cylindrical lens
discharge has the potential advantage of high effi-
20 ns KrF laser
ciency and compactness over a laser-produced-plasma
Fig. 11.221 Schematic diagram of the experimental setup of 13.5 nm device. The uniform high-density plasmas required
optical-field ionization X-ray laser for X-ray amplification can barely by produced by
a conventional electric discharge. Rocca et al. pro-
excimer laser focused at 1017 W/cm−2 (Fig. 11.221), posed [11.1912] and demonstrated [11.1913] a capillary
singly ionized lithium ions were further ionized to fully discharged soft-X-ray laser operating on the 46.9 nm
stripped states, resulting in population inversion with re- transition in Ne-like Ar in 1994. A fast electrical
spect to the ground state of hydrogen ions. A small signal discharge in a capillary was used to excite plasma
gain of 20 cm−1 and a gain-length product of 4 have been columns up to 20 cm in length with a peak current
observed. Subsequently, Korobokin et al. [11.1906] used of 40 kA. Figure 11.223 shows the fast capillary dis-
a plasma waveguide in a LiF microcapillary to improve charge soft-X-ray laser setup. The variation of the
the propagation of the pump pulse and successfully spectra as a function of capillary length is shown in
increase the gain-length product to 5.5. Fig. 11.224. A recently developed compact discharge
On the other hand, Corkum et al. also suggested the occupies a space of only 0.4 × 1 m2 in an optical ta-
use of circularly polarized laser pulses for collisional ble and produces an average output energy of 0.88 mJ
excitation following OFI [11.1907]. Lemoff et al. pro- at a repetition rate of 4 Hz. In two-pinhole interference
posed the specific systems [11.1908] and demonstrated experiments, a high degree of spatial coherence was
lasing at 41.8 nm in eightfold-ionized Xe [11.1909]. In observed by single-pass amplification in a 36 cm-long
this experiments, circularly polarized Ti:sapphire laser capillary. This compact soft-X-ray laser has been used
pulse with an energy of 70 mJ and a duration of 40 fs in a variety areas including plasma physics, material
was focused into a Xe static gas cell to create Pd-like characterization, and the characterization of soft-X-ray
Xe. The intense pump pulse produce the hot electrons optics [11.1914].
which collisionally excite the Pd-like ions to the laser
upper level. Recently, Sebbon et al. reported the sat- 11.12.2 High-Order Harmonics

Survey
Ti: Sapphire laser High-order-harmonic generation (HHG) by the inter-
action of femtosecond high-intensity laser pulses with
a gaseous medium has been extensively studied since it
Al filter
has promising potential for use as a coherent extreme
Spherical X-ray laser ultraviolet and a soft-X-ray (XUV) source as an alterna-
ë/4
mirror tive to soft-X-ray lasers or synchrotron radiation sources.
The harmonic spectrum has a very characteristic shape,
that is, it falls off for the first few harmonics, then shows
Gas cell
a plateau where all the harmonics have the same in-
tensity strength, and finally ends with a sharp cut-off.
A typical harmonic spectrum observed by the interac-
Transmission
grating spectrometer
tion of ultrashort high-intensity pulses with rare gases
is shown in Fig. 11.225. The temporal duration of the
Fig. 11.222 Schematic diagram of the experimental setup of optical- harmonics is considered to be shorter than that of the
field ionization X-ray laser based on electron collision excitation driving laser pulse whose width is typically 100 fs or
Lasers and Coherent Light Sources 11.12 X-ray and EUV Sources 823

less. These spectral and short temporal properties make Theoretical Progress
the high-order harmonics an unique coherent source Theoretical understanding of HHG must be based on
in the XUV region and are opening new application two processes:
fields.
1. a single-atom response in the driving laser field, and
Approach to Shorter-Wavelength Generation 2. a macroscopic response including propagation ef-
Since the demonstration of HHG in rare gases using fects.

Part C 11.12
a KrF excimer laser by McPherson et al. [11.1915] and
a mode-locked Nd:YAG laser by Ferray et al. [11.1916] Both responses must be taken into account to make
in 1987, much effort has been made to extend the har- a comparison between the experimental and theoretical
monic wavelength to a shorter one with various pumping results.
sources. Macklin et al. [11.1917] generated the 109th The emission property of harmonic radiation from
harmonic (7.4 nm) in neon gas excited with a 806 nm a single atom is determined by the induced atomic po-
Ti:sapphire laser. L’Huillier and Balcou [11.1918] ob- larization, or dipole acceleration, which is calculated
served the 135th harmonic (7.8 nm) using a 1 ps Nd:glass from the solution of the time-dependent Schrödinger
laser. In these experiments, ionization of the neutral equation (TDSE). Krause et al. [11.1932] showed that
rare-gas medium limits the achievable wavelength be- the photon energy E max of the highest harmonic in
cause of the low effective interaction intensity due the plateau is give by E max = Ip + 3.17Up , where Ip
to the occurrence of ionization during the interac- is the ionization energy of the nonlinear medium and
tion. Although ions having larger ionization energy Up = 9.33 × 10−14 Iλ2 (eV) is the ponderomotive en-
potentially produce higher harmonics, simultaneously ergy of the electron subjected in the pump laser field
existing free electrons cause a large phase mismatch be- I (W/cm2 ) at a wavelength of λ (µm). In a semi-
tween the pump and high-harmonic waves, resulting in classical picture [11.1933], the physical origin of this
the lowering of cut-off orders. This drawback, which expression is explained in terms of tunneling ionization
arises from the use of ions as a nonlinear medium, of the atom, followed by acceleration of the ionized
was compensated for to some extent with an ultravi- electron in the pump field and recombination with
olet pump source [11.1919]. Nagata et al. [11.1920] its parent ion. During the acceleration by the opti-
and Preston et al. [11.1921] reported the generation cal field, the electron obtains the maximum energy
of the 37th harmonic (6.7 nm) of a 248 nm KrF ex- of 3.17Up . When this electron recombines with the
cimer laser. In those studies with pumping pulses parent ion, the electron release this energy plus the ion-
longer than 100 fs, the shortest wavelength achieved ization energy as a harmonic photon. Figure 11.226
was limited to around 7 nm. More recently, however, shows a semiclassical model of high-order-harmonic
progress of ultrashort-pulse laser technology has en- generation.
abled the use of extremely short pulses with high Since calculation based on the TDSE is quite time
intensity, which allows the circumvention of the lim- consuming, it is very difficult to combine the numer-
itation due to ionization [11.1922, 1923]. That is, ical results of TDSE with the propagation equations.
the effective interaction intensity before the occur- The calculation load is considerably relieved by using
rence of ionization can be increase with the extremely the model of Lewenstein et al. [11.1934, 1935]. This
short pulses. Consequently, harmonic wavelengths well model is based on the strong-field approximation and is
within the water window region was attained, using valid in the region Up > Ip . L’Huillier et al. developed
an ultrashort Ti:sapphire laser operating with a 26 fs a propagation code coupled to the Lewenstein model
pulse duration [11.1924]. With a sub-10 fs Ti:sapphire and successfully described the harmonics characteristics
laser, Spielmann et al. [11.1925] obtained coherent observed in various experiments [11.1936, 1937].
continuum emission shorter than 2.5 nm, which corre-
sponds to a photon energy greater than 0.5 KeV. On Phase Matching
the other hand, a few approaches from the medium In order to increase conversion efficiency and improve
side were reported. Although ions [11.1926, 1927], the spatial quality of high harmonics, phase matching is
molecules [11.1928, 1929] and clusters [11.1930, 1931] essential. It is, however, not easy to satisfy the phase-
have been investigated as nonlinear medium in place of matching condition along the interaction length because,
rare gases, the output property of the harmonics was in contrast with low-order-harmonic generation in the
hardly improved for practical use. perturbative regime, the dipole phase is dependent on
824 Part C Coherent and Incoherent Light Sources

Intensity (arb. units) Intensity


2.5
Mg-like Ar 3 cm
J = 0–1
2
Al-like Ar Ne-like Ar
1.5
3d–3p
Ne-like Ar
1
Part C 11.12

0.5
Plateau Cutoff
0
5
6 cm
4
J = 0–1
Ne-like Ar
3
Mg-like Ar Harmonic order
3d–3p
2
Al-like Ar Ne-like Ar Fig. 11.225 Schematic drawing of typical harmonic spec-
1 trum
0
160
E
140 J = 0–1 12 cm
120 Ne-like Ar
100 Recombination
80
60
40
20 Emission of harmonic photon r
0
46 46.5 47 47.5 48 48.5 49
Wavelength (nm)

Fig. 11.223 Variation of the intensity of the spectral lines in the
Tunneling ionization
neighborhood of 48 nm as a function of capillary length

Coulomb potential
Switch modified by optical field
Capillary
Rogowski coil Fig. 11.226 Schematic drawing of a semiclassical model of
Fast valve
high-order-harmonic generation
Capillary array window
Marx generator +HV To spectrometer
700 kV pump pulse also make the experimental achievement of
phase matching quite troublesome.
Several techniques to control the phase-matching
To vacuum pump conditions have been investigated. Phase matching can
be achieved by controlling the balance of
1. the Gouy phase shift and atomic dispersion
Ethylene glycol [11.1939, 1940]
Fig. 11.224 Schematic illustration of the fast capillary discharge 2. nonlinear phase shift and plasma dispersion
setup [11.1941] or
3. waveguide dispersion of hollow fiber and atomic
dispersion [11.1942, 1943]
the driving laser intensity [11.1938]. Furthermore, in
addition to the medium’s dispersion, nonlinear phenom- A geometrical phase and a dipole phase that have oppo-
ena such as self-focusing and plasma defocusing of the site dispersions are compensated by adjusting the focal
Lasers and Coherent Light Sources 11.12 X-ray and EUV Sources 825

position around a gas jet. This method is extended to low fiber. However, the output energy from the hollow
a loosely focused geometry and successfully improved fiber was restricted to a few nanojoules because only
conversion efficiency and beam quality [11.1944]. The a few millijoules of laser pulse could be introduced due
use of a hollow fiber provides a few advantages for to the limited aperture of the hollow fiber [11.1948].
high-harmonic generation. Due to the flat phase front
of the driving (pumping) laser in the hollow fiber, one Energy Scaling
can avoid undesirable phase modulation of the harmon- For the development of a variety of applications of high

Part C 11.12
ics, which originates from the intensity-dependent phase harmonics (HH), one of the most important issues is
change around the focus [11.1938]. This facilitates the energy scaling. High-energy HH is expected to boost
clear and easy identification of the phase-matching con- new physics in the soft-X-ray region. Takahashi et al.
ditions by adjusting the medium density. The increase report energy scaling of HH in Ar under the optimized
of the intensity–interaction length product would also phase-matched condition [11.1944,1949]. Their scaling
lead to an improvement in conversion efficiency. Fur- method demonstrated a linear increase of harmonic en-
thermore, the use of a hollow fiber results in lower ergy with respect to the geometrical focusing area of
beam divergence and better spatial coherence. Such im- the pump pulse, while keeping an almost perfect spatial
provements are very important for practical applications. profile of the harmonic output. The maximum energy
With this new technique, several groups have reported of the 27th harmonic attained was 0.33 nJ with a con-
harmonic generation. Tamaki et al. first demonstrated version efficiency of 1.5 × 10−5 . The evolution of HH
HHG of a Ti:sapphire laser pulse in an Ar-gas-filled hol- intensities in the spectral region from the 23rd- to 27th-
low fiber and showed hundredfold enhancement around order harmonics was also measured as a function of
the 25th harmonic [11.1945], [11.1946]. Figure 11.227 medium length. The result is shown in Fig. 11.228. The
shows the observed harmonic spectra with and with- solid line shows theoretically fitted intensities for the
out the hollow fiber filled with 5 torr Ar gas. Rundquist 23rd, 25th and 27th harmonics. The coherence length
et al. [11.1942, 1947] also reported phase-matched gen- was estimated to be ≈ 15 cm by fitting the theoretical
eration of the 29th harmonic and improvement of both curves. As was pointed out by Constant et al. [11.1943],
the generation efficiency and the beam quality in the hol- the optimizing conditions for the medium, coherence
and absorption lengths are given by L med > 3L abs and
L c > 5L abs , where L med , L c , and L abs are the medium
Intensity (arb. units)
10
a) 3 cm hollow fiber Harmonic intensity (arb. units)
8 100

10
4

2
1
0 23rd (Labs = 1.16 cm)
25th (Labs = 2.39 cm)
27th (Labs = 6.81 cm)
2 b) 0.5 cm free space
0.1
0 0.1 1 10 100
11 13 15 17 19 21 23 25 27 Medium length (cm)
Harmonic order
Fig. 11.228 Emitted photon number of the harmonics in
Fig. 11.227a,b Observed harmonic spectral distribution argon as a function of the medium length. The solid line cor-
emerging (a) from a 3 cm hollow fiber and (b) in 0.5 cm responds to the calculated photon number for L c ≈ 15 cm
free space. Ar gas pressure is 5 torr with 1.8 torr argon in free space
826 Part C Coherent and Incoherent Light Sources

a) y (mm) a) y (mm)
2
4

1
3
Part C 11.12

2
–1

–2 1
–2 –1 0 1 2
x (mm)
b) Intensity (arb. units)
100 0
0 1 2 3 4
x (mm)
80 b) Intensity (arb. units)
8000
60

40 6000

20
4000
0
–3 –2 –1 0 1 2 3
x (mm) 2000
Fig. 11.229a,b Interferogram of a harmonic beam dif-
fracted by double pinholes separated by 100 µm: (a) fringe 0
image, (b) intensity profile of the interferogram along a hor- 0 1 2 3 4
x (mm)
izontal line passing through the center
Fig. 11.230 (a) Interferogram recorded with a PDI plate
length, the coherence length, and the absorption length, with a 10 µm pinhole. (b) Intensity profile of interferogram
respectively. The 23rd- and 25th-order harmonics satis- along a horizontal line passing through the center
fied the optimized condition for this relation. Therefore,
those orders were saturated under the experimental con- phase matching can realize highly efficient and spatially
ditions. On the other hand, the 27th-order harmonic did well-characterized (nearly Gaussian profile) high-order
not yet satisfy the above conditions, because of low harmonic light [11.1949, 1950]. Several groups have re-
absorption. ported the interferometric measurement of the spatial
coherence of high harmonics [11.1951–1954]. When
Spatial Coherence the macroscopic phase matching is achieved in the
Since HHG is based on nonlinear frequency conversion, hollow fiber or loosely focused geometry, the mea-
the spatial and temporal coherences of high-order har- surements show that the harmonic beams have almost
monics are expected inherently to succeed to those of perfect spatial coherence. Figure 11.229 shows the
the fundamental laser pulse. However, HHG conducted interferogram of the 27th-harmonic beam generated
by use of a tight-focusing geometry in thin gas media did with an Ar-filled hollow fiber pumped with 20 fs,
not allow full phase matching to enhance the coherence. 0.35 mJ Ti:sapphire laser pulses [11.1954]. This in-
Typically multimode components are observed as broad- terferogram was obtained with two pinholes separated
ened peaks in the spectrum or the pedestal of the spatial by 100 µm, while the harmonic-beam diameter was
profiles. Recent studies have revealed that macroscopic measured to be 130 µm. Figure 11.230 also shows the
Lasers and Coherent Light Sources 11.13 Generation of Ultrahigh Light Intensities and Relativistic Laser–Matter Interaction 827

interferogram recorded by point-diffraction interferom- X-rays and matter have been reported by a few groups,
etry, which indicates that the harmonic beam can be such as two-photon ionization of He+ [11.1958], He
considered as a spherical wave within a phase error of double ionization for the autocorrelation of an extreme-
λ/15 [11.1954]. ultraviolet (XUV) pulses [11.1959], the advantages of
high-intensity short-wavelength radiation for Coulomb
Applications explosion imaging [11.1960], and the ionization of clus-
In addition to applications in atomic physics [11.1955], ter targets. These research field can be expected to open

Part C 11.13
high harmonics have been used for solid-state spec- a new area in high-intensity physics.
troscopy [11.1956] and plasma diagnostics [11.1957]. Furthermore, coherent XUV and X-ray pulses are
High intensity of high harmonics is also expected to not only useful owing to their short wavelengths, but
give rise to nonlinear phenomena in the XUV region. As are also important due to their potential to produce
described above, Takahashi et al. [11.1944, 1950] gen- electromagnetic radiation in the range of attoseconds.
erated a peak power of 130 MW at 62.3 nm in 0.6 torr High-order harmonics have been expected to be the
Xe and 10 MW at 30 nm in 2 torr Ar. When these source of attosecond pulses [11.1961, 1962]. Recently,
harmonic pulses are focused with multilayer mirrors, Hentschel et al. [11.1963] demonstrated the genera-
the focused intensity will reach 1014 W/cm2 , which is tion of isolated soft-X-ray attosecond pulses and their
high enough to cause nonlinear interactions. Theoret- temporal characterization by a novel cross-correlation
ical predictions of nonlinear interaction between soft technique using intense few-cycle visible laser pulses.

11.13 Generation of Ultrahigh Light Intensities


and Relativistic Laser–Matter Interaction
Modern laser technologies allow the amplification of of the laser material. Hence, a short pulse cannot be am-
short laser pulses to energies of some tens of kJ. Addi- plified efficiently. The chirped pulse amplification (CPA)
tionally, ultrashort pulses containing only a few optical
cycles can be generated. By merging these techniques
nowadays focused laser beams can reach unprecedented
intensities in the range of 1021 W/cm2 and will reach
even higher values in the near future. At these inten-
sities the electric and magnetic field strength is many
orders of magnitude higher than those that will ever be
possible in a static generation scheme. By applying these
fields to a target it becomes possible to gain access to
a new interaction regime of light and matter: relativis-
tic optics. This opens a new wide area in experimental
science where classical optics meets plasma dynam-
ics, relativistic quantum mechanics, and high-energy
physics. Chirped pulse
Compressor
11.13.1 Laser Systems for the Generation
of Ultrahigh Intensities Amplifier

Amplification of Ultrashort Pulses Stretcher


to High Energies
For ultrashort pulses the energy density of light at the Fig. 11.231 The CPA principle. An ultrashort pulse gener-
surface and in the volume of all the optical elements ated in a mode-locked laser is stretched by adding a spectral
is limited by the onset of nonlinear effects and laser phase that group delay different wavelengths of the pulse.
damage due to the high peak power. Moreover, in a laser After amplification retaining the pulse spectrum and chirp
amplifier the energy extraction efficiency is a function of the pulse is recompressed to its original length, resulting in
the ratio of the energy density and the saturation fluence ultrahigh peak power
828 Part C Coherent and Incoherent Light Sources

technique [11.1964] circumvents this difficulty. The of the arrangement. Section 12.1.3 contains a detailed
principle of CPA is depicted in Fig. 11.231. Ultrashort description of these devices.
pulses contain a broad spectral bandwidth according to For ultrahigh-peak-power lasers a maximum stretch-
their Fourier transformation (see Chap. 12). This fact ing/compression factor, i. e., the ratio of stretched pulse
enable the possibility to add a phase shift to different length to bandwidth limited pulse length is required in
frequencies or wavelengths of the laser pulse just after order to maximize the fluence in the amplifier chain. The
its generation in a mode-locked laser cavity. The result stretching factor depends on the line density of the grat-
Part C 11.13

is a stretched pulse containing a chirp, i. e., the pulse du- ings, the center wavelength, and the bandwidth of the
ration is no longer bandwidth limited. The lengthened pulse. Very long stretching factors of 10 000 or more are
pulse has accordingly a lower peak power. It can be am- required for most broadband rare-earth-doped laser ma-
plified much more efficiently and compressed to a very terials in order to allow fluences in the amplifier close to
short pulse afterwards by adding a spectral phase with or above the gain-saturation fluence.
an opposite sign to that introduced by the stretcher. If the grating distance is chosen in this way, such that
After the invention of the CPA technique tremen- the unclipped spectral bandwidth is twice the spectral
dous progress in the development of ultrashort pulse full width at half maximum (FWHM) of the pulse, the
lasers towards higher peak power has been witnessed. maximum stretched pulse length τmax is only a function
Nowadays, terawatt (TW) laser pulses can be produced of the grating size L:
using tabletop laboratory-scale laser systems that op-
L
erate at repetition rates of 10 Hz or higher. Whereas, τmax = 2 cos (α) , (11.205)
even higher power up to the petawatt (PW) can be c
generated by flashlamp-pumped lasers that have factory- where cos α is a factor according to the diffraction angle
building sizes, like the first PW laser, that was realized α of the grating and has a maximum of unity in the un-
in 1999 [11.1965]. The CPA technique is common to all realistic case of a diffracted beam parallel to the grating
of these devices. surface. The factor of 2 refers to the Littrow case, i. e.,
Because pulse stretching and compression are re- the input and diffraction angle being equal. The latter
lated to each other and are normally based on the same normally maximizes the grating diffraction efficiency.
principle, the stretcher and compressor are treated here For holographic metal-coated diffraction gratings with
as a stretcher–compressor pair (SCP). Pulse stretching near-rectangular groove shapes it has been shown that
naturally occurs in the vicinity of dispersion. Hence, an optimum diffraction efficiency of a metal grating at
the propagation of pulses in dispersive media always wavelength
√ λ can be achieved for a grating constant of
leads to pulse stretching. In order to keep the required about 2λ [11.1967], which results in a Littrow angle of
space and size of optical elements as small as possible 45◦ . This leads to a minimum grating size for an SCP of
highly dispersive optics, i. e., gratings will be used. Nev- about 24 cm if a femtosecond pulse has to be stretched
ertheless other elements such as prisms, grating prisms to 1 ns. Passing a stretcher or compressor setup again
(so called grisms), fibers and chirped fiber Bragg grat- can, in principle, increase the stretching factor, but in-
ings as well as chirped mirrors can be applied. Here troduces losses that are most often acceptable for the
we limit ourselves to the simplest case of flat reflec- stretcher but not for the pulse compressor.
tive phase gratings, because these offer the largest group Very large grating distances and hence long stretched
delay. pulses require a similar accuracy for the compensation
The principle of pulse compression with identical of dispersion by a well-matched stretcher and compres-
parallel gratings was first described by Treacy [11.1966]. sor as in the case of ultra-broadband fs pulses, because
A pulse is diffracted by a grating, angularly split into higher-order dispersion terms increase together with the
its different wavelengths and propagated to the second second-order term. Because most often aberrations of
parallel-aligned grating. The second grating removes the the telescope optics cannot be tolerated, aberration-free
angular modulation, i. e., redirects all wavevectors of all-reflective designs like the Öffner triplet are ap-
the different wavelets into the same direction. If all the plied [11.1968]. In special cases aberrations introduced
waves are treated as plane waves, the introduced lat- by the stretcher may help to compensate for laser-
eral shift can be neglected. For a real, limited beam material dispersion in the amplifier chain [11.1969].
size the same device of parallel gratings has to be used The required grating sizes for the compressor of
once more in order to combine the wavelets again spa- a high-energy laser system is ruled by the generated
tially. As a side effect this doubles the stretching factor group delay in order recompress the pulse and the size
Lasers and Coherent Light Sources 11.13 Generation of Ultrahigh Light Intensities and Relativistic Laser–Matter Interaction 829

Fig. 11.232 (a) Capability of laser materials for energy stor-


age and generation of high energy pulses. The inverse a) Inverse of saturation fluence Fsat–1 (J–1 cm2)
saturation fluence is plotted against the fluorescence life- 101
YVO GdVO
time. For a higher gain amplified spontaneous emission Cr:YAG SFAP
YAG BFAP
(ASE) become an issue whereas for lower gain damage Ti:Sa
YAlO YLF
limits efficient energy extraction. Effective pumping will be 100 Cr:MgSiO
YVO SFAP
useful if the fluorescence lifetime exceeds a certain limit.
ASE issues

Part C 11.13
The limits are marked with dashed lines. (b) Capability of Cr:LiSAF 1 FAP
Damage issues Glass 2
laser materials for energy storage and generation of high 4 3
10–1
peak power. The inverse saturation fluence multiplied by 5 6 Ruby
1 KGW, KYW 5 SSO 7
minimum possible pulse width plotted against fluorescence 2 YAG 6 LSO Cr:BeAlO
3 BOYS 7 SYS GCOB
lifetime τ. Differently doped materials are marked with 4 YSO Glass
10–2
different colors CaF2
Yb doped
Nd doped
required to fit the compressor to the beam diameter. Be- Transition metal doped Diode pumping
fore compression the laser beam has to be expanded to 10–3 –3 –2 –1
10 10 10 100 101
reduce the fluence in the beam to an amount well below Fluorescence lifetime ôf (ms)
the damage threshold of the compressor optics, partic-
ularly the gratings. For a metal-coated grating damage
thresholds may reach the 0.5 J/cm2 level [11.1967] for
b) Inverse product of saturation fluence and
half-ps pulses, but will normally be less than 0.25 J/cm2 . minimum pulse duration (Fsat t min)–1 (J–1 s–1cm2)
In the compressor setup these fluences result in intensi- 1015
ties that are well above the onset of nonlinear effects in Ti: Sa Maximum performance (at 1 µm)
air at normal pressures. In order to prevent the pulse
from self-focusing and self-splitting into white-light 1014
filaments, pulse compression has to be performed in Cr: LiSAF
a vacuum vessel. 13 Cr: MgSiO
10 Cr: BeAlO
In the region of fs to ps pulses the damage thresh- GdVO
old for metal coatings is nearly independent of pulse YVO Glass KGW
YAlO KYW
duration, in contrast to dielectrics where the main dam- YLF SFAP
1012 YAG CaF
YAG
age mechanism is linked to nonlinear absorption effects.
BOYS Glass GCOB
For pulses longer than 100 fs dielectric gratings may
substantially improve overall performance [11.1970]. 1011 Ruby
Yb doped
Damage thresholds two to four times that of gold-coated Nd doped
gratings are reported. These dielectric phase gratings on Transition metal doped Diode pumping
1010 –3 –2 –1
top of a multilayer mirror can, in principle, show a 100% 10 10 10 100 101
diffraction efficiency to the minus-first order [11.1971]. Fluorescence lifetime ôf (ms)
Therefore they are favored in high-energy high-peak-
power laser systems.
The peak power of a laser system is limited mainly two 350 mm-wide gold-coated gratings with the help of
by the possible sizes of the diffraction gratings. A work- a six-axis piezo-driven mount.
around is to add identical smaller gratings to a mosaic
grating or tiled grating. The smaller grating tiles have Laser Materials for High Peak Power
to be coherently phased together in order to make them A crucial issue conceiving a high-peak-power laser sys-
work like a single one. Using this technique to build tem is the choice of the gain material. Broad band width
a compressor opens the way to further power scaling and a high cross section for stimulated emission are
of high-peak-intensity lasers. Compression of pulses required. Due to the limited peak power of the pump
to 650 fs with a tiled grating replacing a meter-sized source a long fluorescence lifetime for energy storage
grating in a high-energy laser system has already been is desired. At higher fluorescence lifetimes either the
demonstrated [11.1972], as well as pulse compression of emission cross section, or the gain bandwidth, or both
a chirped 2 ns pulse down to 150 fs [11.1973] by phasing decrease. For efficient amplification the extracted laser
830 Part C Coherent and Incoherent Light Sources

pulse energy density has to be close to the saturation three options for pumping exist: flashlamps, lasers, and
fluence of the gain medium. diode lasers. Diode lasers are treated separately because
Figure 11.232 illustrates the possibility of generating no enhanced additional pumping is required for them,
high peak power out of some established laser mater- providing a stabilized current is sufficient.
ials. The inverse of the product of the saturation fluence So far the flashlamp is the cheapest generator for
and the shortest pulse duration indicates the capability a high pump photon flux. In the past flashlamp-pumped
of a laser material for high amplification at maximum solid-state lasers have been scaled to 20 kJ pulse en-
Part C 11.13

bandwidth. Assuming Gaussian-shaped gain spectra the ergy in a single beam. Such systems are based on
correlation between the emission cross section, band- schemes where bundles of meter-size flashlamps pump-
width and fluorescence lifetime of a laser material is ing several Nd-doped glass discs arranged at Brewster’s
given by angle in the laser beam path as sketched in Fig. 11.233.
√ For fusion lasers like the National Ignition Facility in
c20 1 ln 2
σem = √ (11.206) the US (NIF) [11.1975], Laser Megajoule in France
4πn 2 ν2 τf ∆ν π (LMJ) [11.1976] or Gekko in Japan [11.1977] several
with c0 the velocity of light in vacuum, n the refractive such beam lines are bundled together to form megajoule
index, h Planck’s constant, ν the center frequency, τ f the laser facilities. Such beam lines were the first with the
fluorescence lifetime, and ∆ν the bandwidth (FWHM). capability to generate petawatt laser pulses [11.1965].
Applying the time–bandwidth product for Gaussian line- Typical for this kind of lasers are a double-pass main
shape a criteria for the generation of high peak power amplifier and a single-pass booster amplifier section.
at a corresponding fluorescence lifetime depending on The drawback of flashlamp pumping is the low ef-
the laser wavelength lambda and the refractive index n ficiency of this scheme. Pump photons are not only
is obtained generated at the absorption wavelength of the laser
τf (λ[µm])3 [cm2 ] material but also at wavelengths not involved in the
≤ 4.26 × 109 . (11.207) lasing process. This low efficiency results in sub-
tp Fsat n2 [J] stantial heat left inside the laser materials, which
Here the saturation fluence Fsat is given by are themselves poor heat conductors. The maximum
Fsat = hν/σem . repetition rate of this disc configuration scales with
In Fig. 11.232 suitable materials for amplification the inverse square of the beam diameter. Amplifiers
to a high energy level are mapped. Furthermore, there with beam diameters of some 10 cm can be oper-
is an optimum region between high gain and low gain, ated at repetition rates of some shots per day only.
where amplified stimulated emission and damage issues, With these systems scientific investigations of plasma
respectively, are likely to occur. effects are extremely difficult and expensive. For Nd-
Recently, it was observed that cryogenic laser doped glasses the gain bandwidth limits the shortest
materials may show enhanced performance. Either pulses to about 400 fs. To generate 100 TW to PW
spectroscopic parameters and thermal behavior can peak power pulses, energies in the 100 J range are
be improved by cooling to liquid-nitrogen tempera- needed, which require large amplifiers. Nevertheless,
tures [11.1974]. Ti:Sapphire for instance gain, higher using these lasers for pumping an OPCPA (see below)
efficiency and thermal conductivity. Quasi-three-level opens the door for ultra-broadband amplification of few-
systems represented by the Yb-level system show higher
emission cross sections and additionally reduced absorp-
tion at the laser wavelength, because population of the Flashlamps Flashlamps
low laser level is suppressed. Spatial
filter
Laser Amplifier Schemes for High Peak Power
Except some examples of high-energy excimer lasers
and upcoming free-electron lasers for the generation of
Flashlamps Input Flashlamps
high peak power at very short wavelengths typical sci-
entific lasers are based on solid-state lasing materials Fig. 11.233 Typical flashlamp pumped slab amplifier con-
as presented above, all of which are pumped opti- figuration. The seed pulse is injected at the spatial filter
cally. Because a high flux of pump photons is needed between a double-pass section and a single-pass booster
to invert the energy-level population significantly only amplifier
Lasers and Coherent Light Sources 11.13 Generation of Ultrahigh Light Intensities and Relativistic Laser–Matter Interaction 831

cycle pulses to the 10 J level with reasonable repetition


rates [11.1978]. a) b)
Using laser diodes as the pump source helps to
relieve some of these difficulties because their emis-
sion spectrum is much narrower and can be fitted to
the absorption line of the laser-active medium. Con-
sequently less energy is wasted and less heat is left

Part C 11.13
inside the laser active medium. However, high-power
diodes with energy-conversion efficiencies up to 75%
and continuous-wave output in the 100 W range are
only available in the red and near-infrared spectrum. c) d)
These diodes are based on double heterostructures of
ternary and quaternary semiconductors incorporating
GaAs. This spectral range is preferred for pumping rare-
earth-doped laser materials, where Nd and Yb are most
favored. Broadband gain materials including transition
metals such as Cr:LiSAF will attract more interest if
suitable diodes providing high brightness are developed. e) f)
Today diode-pumped infrared frequency-doubled lasers
are used to pump Ti:sapphire, the laser material able
to amplify the widest spectrum and hence the shortest
pulses.
The direct diode-pumped amplification of 150 fs
pulses to the joule and 10 J level has already been
shown by pumping an Yb-doped fluoride-phosphate
glass at 940 nm [11.1979, 1980] with the edge-cooled g) h)
disc arrangement shown in Fig. 11.234a.
To accomplish experimentalists’ demands for higher
repetition rates advanced cooling technologies have to
be developed even for diode-pumped solid-state lasers
(DPSSL). Figure 11.234 shows a variety of DPSSL
pumping schemes with different cooling architectures. Gas flow
Laser beam
In slab lasers, where the various pump schemes de-
Pump beam
picted in Fig. 11.234b–d are employed, one dimension
Heat removal
is used to provide a small distance for heat removal.
They differ in the way in which pump light is pro- Fig. 11.234a–h Amplifier schemes for diode pumping. Edge cool-
vided. Expanding this idea to two dimensions results ing: (a) discs – conductive cooling (b) transverse diode-pumped
in the cladding pumped fiber amplifier (Fig. 11.234g), structured slab and (c) transverse diode-pumped slab. Water cool-
which is not or only radiatively cooled like the heat ing: (d) zigzag slabs and (e) thin discs. No cooling: (f) heat-capacity
capacity lasers (Fig. 11.234f), which are able to run lasers and (g) fiber amplifiers. Gas cooling: (h) thin-disc assemblies
as long as the temperature does not reach a certain
level. These lasers provide bursts of pulses. Thin disc By putting several thin discs together and using the
lasers (Fig. 11.234e) allow a very high average power amplifier slab interspace for gas cooling, as in the archi-
and can produce very good beam profiles but are dif- tecture sketched in Fig. 11.234h, the gain and absorption
ficult to scale to larger beam diameters and higher equals that of the thick disc but efficient cooling is
pulse energies. A compromise is the use of a thicker enabled. A diode-pumped laser of this type was devel-
disc at a moderate repetition rate in the same con- oped at the Lawrence Livermore National Laboratory
figuration. The thicker disc does not require multiple in the US. It is called Mercury [11.1981] and allows
pump-beam passes for full absorption and provides an output of 65 J, the highest ns pulse energy from
a larger single-pass amplification than the thin-disc a single DPSSL at a repetition rate of 10 Hz so far
amplifier. reported.
832 Part C Coherent and Incoherent Light Sources

The long propagation length in a fiber that con- distances of the pulse in the active medium the seed pulse
fines the laser light field to the doped and amplifying itself has to be converted into a top-hat profile starting
core allows high amplification factors in a single pass from a Gaussian. A simple method to implement this is
and optical-to-optical efficiencies close to the theoretical by diffraction at a serrated aperture [11.1982].
limit given by the quantum efficiency. For TEM00 -mode Because a top-hat beam unlike the Gaussian changes
radiation the maximum pulse energy is limited to some its profile while propagating it has to be relay imaged to
mJ for CPA. Nevertheless, average powers from sev- successive optical elements of the laser system to avoid
Part C 11.13

eral 100 W to the kW region are possible. To reach hot spots and laser damage. In high-power laser systems
a high extraction efficiency for the low-energy seed relay imaging is often combined with beam expanders
pulses provided by fs oscillators multipass amplifiers and spatial filters [11.1983].
or regenerative amplifiers are adopted. Multipass ampli-
fiers can be found with a variety of geometries. All pulse Broadband Optical Parametric Chirped Pulse
parameters, such as the polarization or propagation di- Amplification
rection, can be used to separate pulses from successive Alternatively instead of conventional laser amplifiers
passes and finally for out-coupling. a parametric amplification process (OPA) can be used
The regenerative amplifier is a seeded oscillator with for the generation of high-energy broadband pulses. In
an active element, in most cases a fast switching Pock- this second-order nonlinear interaction a pump photon
els cell, that allows the extraction of the amplified pulse is split into a signal and an idler photon. This process
when the gain of the active medium is saturated. It ben- is the reverse of sum-frequency generation. Energy-
efits from a stability that stems from gain saturation conservation demands that the sum of the signal and idler
and beam quality that is ensured by successive spatial frequencies equals the pump frequency. Additionally,
filtering in the laser cavity. The drawbacks of regenera- fulfilling momentum conservation ensures coherence
tive amplifiers are pre-pulses produced by leakage from of the involved waves while propagating through the
the cavity in round-trips before extraction and long path nonlinear medium. The latter is known as phase match-
lengths in dispersive material that has to be compensated ing. The nonlinear medium has to be a crystal in order
by the SCP of a CPA system. to show second-order nonlinearity and achieve phase
The last section of a high-power laser amplifier sys- matching. The phase-matching condition also deter-
tem is a booster amplifier with a low number of passes or mines the wavelengths of the signal and idler waves.
one pass only. In order to extract the energy with high- For a certain direction of pump, signal, and idler
efficiency, saturation fluence has to be reached across the waves only one combination of wavelengths can be
full beam diameter. The result is a so-called top-hat beam generated. In order to allow broadband amplification
profile with a uniform fluence in the center and a steep of a signal input wave using a narrow-band pump the
fluence rise at the edge. In gain media with a long propa- different idler wavelengths should have different di-
gation distance this may be achieved automatically after rections in the crystal. This principle is illustrated in
some distance and the length were uniform aperture fill- Fig. 11.235 and is called optical chirped pulse amplifi-
ing is not guaranteed hardly affects the overall efficiency cation (OPCPA) if the signal beam is a chirped stretched
of the amplifier. For amplifiers with short propagation pulse [11.1984–1987].
With the OPCPA scheme, energy can be transferred
from a narrow-band nanosecond pulse to a stretched
ks ki broadband signal pulse. The problem of amplification
of ultrashort pulses is thereby split into the task of
amplification of high-energy laser pulses and the task
kp
of implementation of broadband OPA. Comparing the
OPCPA with a conventional laser-pumped CPA several
Fig. 11.235 Scheme to achieve broadband optical paramet- advantages can be realized. Firstly no energy is stored
ric amplification. In order to achieve broadband signal in the nonlinear crystal and, except parasitic absorption,
amplification in a parametric nonlinear optical process us- no energy is lost in the crystal, which results in no heat
ing a narrow-band pump different idler wavelengths have being produced in the process. This fact allow easy high-
different propagating directions in a crystal to fulfill the repetition-rate scaling of the amplifiers without phase
phase-matching condition while all signal waves propagate distortions by thermal effects. Because no resonance to
collinearly energy levels of a dielectric medium is required, very
Lasers and Coherent Light Sources 11.13 Generation of Ultrahigh Light Intensities and Relativistic Laser–Matter Interaction 833

large band widths at any center wave length can be gen- at a fixed fluence, which reduces the required crystal
erated. It was shown that pulses shorter than 10 fs can length, with the advantage of increasing the amplifica-
be amplified. Using crystals with high nonlinear optical tion bandwidth without changing the crystal orientation.
coefficients like the most prominent crystal BBO and at More requirements may arise at different wavelengths
sufficient intensities a single pass can provide an am- involved, like absorption, or second-harmonic genera-
plification of the signal by many orders of magnitude. tion from the signal or idler beams, amongst others.
Regenerative amplifiers are not needed and the problem Nevertheless, OPCPA is the technique that allows

Part C 11.13
of pulse leakage from them disappears. Amplification the implementation of an ultrashort pulse option to all
lasts only as long as the pump passes the crystal and coherent high-energy light sources that emit pulses in the
therefore pre-pulses and post-pulses as well as back- nanosecond and picosecond range and transfers them to
reflected pulses are not amplified any more and higher an ultrahigh-peak-power laser system. A 200 TW 45 fs
pulse contrasts are possible with the OPCPA technique. laser system was recently demonstrated [11.1988] based
Lastly the amplified signal beam is an analog of the on OPCPA in a large-aperture KDP crystal. These crys-
input signal and unwanted phase distortions of the high- tals are used for Pockels cells and frequency converters
energy pump are carried away with the idler beam like in fusion laser systems and can be grown with meter-size
the different k vectors in Fig. 11.236. apertures. This in principle allows multi-petawatt power
In order to use all of these advantages a careful de- scaling.
sign of OPCPA is required. For instance if an OPCPA
stage is driven to its maximum amplification and the High Demands on Pulse Preparation
process starts to saturate, the impact of intensity varia- for Advanced Experiments
tions of the signal to the output is reduced but intensity The acceleration of electrons and protons by a laser
variations of the pump are transferred to the amplified requires light intensities on the order of 1020 W/cm2 ,
beam. Additionally, signal and idler waves are generated which is many orders of magnitude above the onset of
starting from noise, a problem similar to the amplified nonlinear effects and atom ionization, which results in
spontaneous emission (ASE) in a conventional laser am- Coulomb explosion even in low-density targets such as
plifier. To minimize this effect a pump pulse length no gases, triggered by lower intensity background radia-
longer than the seeding signal pulse and their perfect tion of the laser. Experiments are strongly affected by
synchronization is required, which is challenging for ps this pre-pulse laser-target interaction [11.1989]. To pre-
pulses. Contrariwise ps pulses offer higher intensities vent the target from being destroyed before the main part
of the laser pulse arrives, laser output has to be cleaned
from its leading pedestal. A typical laser pulse character-
log intensity istic is shown in Figure 11.236. The long-term pre-pulse
pedestal results from ASE of the laser active material,
Main pulse whose duration is closely linked to its fluorescence life-
time. Additionally, regenerative amplifiers that are often
used as the first devices in the amplifier chain, always
have a certain leakage of pulses from preceding round-
Uncompensated spectral modulations trips. The pulses are again amplified in successive mul-
Amplified leaking pulses tipass and booster amplifiers, generating high-energy
pre-pulses on target. Finally, non-bandwidth-limited
pulse recompression based on material dispersion, wave-
ASE pedestal length clipping, aberrations in stretcher and compressor
setups and uncompensated higher-order dispersion
terms result in pre-pulses and pedestals as shown in
Sect. 12.1.2 for frequency-domain-filtered short pulses.
–10–6 –10–9 –10–12 0 Numerous methods are used to remove this un-
Time (s)
wanted pre-pulse laser light. Primarily, the total
Fig. 11.236 Typical pulse contrast characteristics. The main amplification is split into stepwise amplification with ad-
femtosecond laser pulse is typically preceded by ampli- ditional possibilities for time-domain and spatial pulse
fied stimulated emission (ASE), amplified pre-pulses and filtering. For this purpose fast Pockels cells [11.1990]
uncompressed chirp and spatial filters, which are often combined with
834 Part C Coherent and Incoherent Light Sources

beam expanders, are applied. Spatial filters and aper- pared to classical, even classical nonlinear optics. At
tures prevent spontaneously emitted fluorescence light intensities of 1013 –1015 W/cm2 matter becomes ion-
from propagation to the subsequent amplifiers. These ized and the high intensity laser pulse interacts with
measures can often improve pulse contrast ratios con- a dynamically evolving plasma where the dominant
siderably [11.1991]. mechanism for the interaction of light and matter is the
Nonlinear optical effects that favor high inten- interaction with free electrons.
sities can be used as well. Examples of the latter In classical optics the interaction of light and matter
Part C 11.13

case are saturable absorbers and laser pulse switched is described in the following way: the electric field of
gates. The OPCPA inherently embodies such a gate if an electromagnetic wave exerts a force on the bound or
a rectangular-shaped pump pulse is used. Therefore pre- free electrons, which then oscillate with the frequency of
pulse suppression in the OPCPA [11.1992] can be as the wave. The dependence of the oscillating polarization
high as its gain. induced in the material by the motion of the electrons
Saturable absorbers and self-phase-conjugating mir- on the driving electric field then yields the linear and
rors are used for nanosecond laser systems. In the case nonlinear optical constants of the material. Although
of a chirped pulse amplification system these techniques this picture is inherently classical it also provides the
require pulse compression before and stretching after fil- general idea of a quantum-mechanical description of
tering. This limits their application to low-energy pulses light–matter interaction.
or prohibits their use if very long stretching factors are This classical description of light–matter interac-
needed. tion is based on two assumptions, which are valid for
Nonlinear effects can also be used after final pulse sufficiently low light intensities:
recompression. One possibility is frequency conversion
by second-harmonic generation. Another pre-pulse sup- 1. the force exerted on the electrons by the magnetic
pression method with high efficiency and low loss is the field of the electromagnetic wave may be neglected.
usage of a plasma mirror [11.1993]. Because the laser 2. The speed of the oscillating motion of the electron
has to be focused anyway a perfectly transmitting di- is small compared to the speed of light.
electric medium is placed near the focus of the beam.
The leading edge of the pulse is transmitted until the The breakdown of these two approximations marks the
intensity reaches the ionization threshold. At this step onset of relativistic optics, which is based on a fully
a plasma is generated with increasing electron density. relativistic description of the interaction of an electro-
The plasma occurs on a time scale that does not allow magnetic wave with matter.
it to expand. If the plasma frequency matches the laser
frequency this plasma acts as a perfect mirror and the Relativistic Motion of an Electron
main pulse is reflected to the target. With a single plasma in an Electromagnetic Wave
mirror the contrast ratio for petawatt-class lasers can be We first consider the equation of motion of a free electron
improved by factors of about 100 [11.1965]. in the field of an electromagnetic wave
Experiments with lasers at ultrahigh intensities re- d    
quire the focusing of a high-peak-power laser onto γ m ṙ = −e E + ṙ × B , (11.208)
dt
a very small spot. Phase distortions in the beam
line can increase the minimum spot size in the fo- where t is the time, m the electron rest mass, ṙ the
cal plane considerably. Adaptive mirrors are used to velocity of the electron, e the elementary charge, E the
correct phase fronts [11.1994]. Closed-loop systems electric, B the magnetic field of the electromagnetic
allow near-diffraction-limited focusing of ultrashort wave, and
pulses [11.1995,1996]. These techniques today allow in- 2
− 1
tensities in the range of 1020 –1021 W/cm2 with terawatt γ = 1 − ṙ /c2
2
,
and petawatt laser systems.
where c is the speed of light in vacuum. For a plane
11.13.2 Relativistic Optics electromagnetic wave of frequency ω and wavenum-
and Laser Particle Acceleration ber k = ωc propagating in the z-direction we insert
E = E0 cos (ωt − kz). Since ∇ × E = −∂ B/∂t we ob-
The interaction of light and matter at intensities of tain: |B| = |E| /c. Before solving (11.208) we introduce
1020 –1021 W/cm2 changes considerably when com- the normalized quantities: tˆ = ωt, ẑ = zω/c, β = ṙ/c and
Lasers and Coherent Light Sources 11.13 Generation of Ultrahigh Light Intensities and Relativistic Laser–Matter Interaction 835

eE 0
a0 = mωc . Then we rewrite (11.208) in components as- Θ = tˆ − ẑ:
suming linear polarization of the electric field in the
x-direction: x̂ = a0 (1 − cos Θ) ,
ŷ = 0 ,
d    
(γβx ) = a0 (1 − βz ) cos tˆ − ẑ , a02 1
dtˆ ẑ = Θ − sin 2Θ , and
d   4 2
γβ y = 0 ,

Part C 11.13
a 2
dtˆ γ 2 = 1 + 0 sin2 Θ . (11.210)
d   2
(γβz ) = a0 βx cos tˆ − ẑ . (11.209)
dtˆ The motion of the electron is displayed in Fig. 11.237
in two different coordinate systems:
Although (11.209) may be solved for more-general ini-
tial conditions we give here the solution for an electron 1. the laboratory frame and
initially at rest in the origin of our coordinate system, 2. the average rest frame of the electron, which is
i. e., r(0) = 0 and ṙ(0) = 0, with the phase parameter a coordinate system co-moving with the electron in
the ẑ -direction, where the coordinate ẑ is given by
ẑ = ẑ − a02 /4Θ.
a) x (c/wL)
4 It is immediately apparent that the motion of the electron
in the fully relativistic case is quite different from the
3
classical picture, where a solution of (11.208) is obtained
for γ = 1 and B = 0.
The electron oscillates, as in the classical case, peri-
2 odically in the x̃-direction, the direction of polarization
of the oscillating electric field. However, unlike in the
1 classical case the electron is also accelerated in the
ẑ-direction, the propagation direction of the electromag-
netic wave. The magnitude of the electron motion is
0
0 5 10 15 20 25 governed by the parameter a0 , the dimensionless electric
z' (c/wL) field strength [11.1997]. In the classical picture γ = 1,
b) x (c/wL) B = 0 which of course becomes incorrect at high ve-
4 locities; the condition a0 = 1 would correspond to an
3.5 electron that acquires a maximum oscillation velocity of
3 ṙ = c. The condition a0  1, therefore corresponds to
2.5
the classical case of |ṙ|  c while a0 1 describes the
extreme relativistic motion of the electron. In practical
2
units a0 is given by:
1.5
1 Iλ2
a02 = (11.211)
0.5 1.37 × 1018 W cm−2 µm2
where I is the light intensity and λ its wavelength. For
–0.4 –0.2 0 0.2 0.4
z' (c/wL)
optical wavelength where λ ≈ 1 µm intensities above
I ≈ 1018 W/cm2 are therefore called relativistic intensi-
Fig. 11.237 (a) Trajectories of a free electron in a travel- ties. In the extreme relativistic case a0 1 the distance
ing electromagnetic wave for different laser field strengths the electron travels in ẑ-direction during one electric
a0 = 1 and a0 = 2 calculated for the initial conditions field oscillation is much larger than its excursion in the
θin = 0 and βz0 = 0 in the laboratory frame. (b) The tra- x̂-direction, and a complete reversal of the conditions
jectories in the moving frame of the electron (indicated by found in the weakly relativistic case a0 < 1 occurs. The
the primed coordinate) exhibit the characteristic figure-of- acceleration of electrons in the propagation direction of
eight movement. Laser field strength and initial conditions the electromagnetic wave appears to be in contradic-
corresponding to (a) were used tion to the well-known fact derived from energy and
836 Part C Coherent and Incoherent Light Sources

momentum conversation that free photons cannot accel- This force will act on particles that oscillate in spatial re-
erate free electrons. In fact if a light pulse is considered gions where the laser intensity is high and push them into
the electron acquires kinetic energy in the rising part of regions of lower laser intensity. It is instructive to con-
the pulse and looses it again to the electromagnetic wave sider the weakly relativistic limit of the ponderomotive
in the falling part of the pulse. After the pulse has left, force. With the definition of a0 we find for γ  − 1  1:
the electron experiences a shift in the propagation di- e2
rection of the pulse but has not acquired a net energy Fp = − ∇ E 02 (r) . (11.215)
4mω2
Part C 11.13

in agreement with the conservation laws for energy and In the classical limit this constitutes the gradient of the
momentum. If, however, the field of the electromagnetic time-averaged kinetic energy of the electron oscillating
wave is suddenly switched off while the electron moves in the laser field [11.1998].
in the propagation direction the electron cannot give its Another way to look at the ponderomotive force is
energy back to the field and maintains its energy ac- to view regions of high laser intensity as regions of
quired from the field. The switching of the field may be high electromagnetic energy density W = ε0 E2 (r, t)/2,
achieved, i. e., by shielding the field in a steep plasma which represents a pressure pushing the electrons from
gradient or by a guiding channel. regions of high pressure to those of low pressure.
The second interesting feature of the solution of the
equation of motion (11.209) is the anharmonic oscillat- The Optical Properties of a Relativistic Laser
ing motion of the electron in the x̂- and ẑ-direction best Plasma and Relativistic Channeling
seen in the co-moving frame (Fig. 11.237b). This means When an intense laser pulse at relativistic intensities
that the electron radiates not only at the frequency of propagates through a gas consisting of atoms with low
the diving electromagnetic wave but also emits other atomic number, such as hydrogen or helium, the rising
frequencies. While for a0 < 1 the spectrum contains part of the laser pulse fully ionizes the gas and the laser
essentially the even (polarized in the ẑ-direction) and pulse interacts with a fully ionized plasma. For example
odd (polarized in the x̂-direction) harmonics, the spatial helium is fully ionized already at an intensity of a few
and spectral emission pattern becomes very complex for times 1016 W/cm2 while relativistic intensities usually
higher intensities (a0 > 1). This phenomenon is called exceed 1018 W/cm2 . The dielectric constant of a fully
nonlinear Thomson scattering and has been observed ionized plasma is given by
experimentally.
ω2p
εr = 1 − , (11.216)
The Ponderomotive Force ω2
2
The total energy of the electrons driven by the electro- where ω2p = εe0 γnme and n e is the electron density.
magnetic field of a laser is given by Collisions have been neglected here which is a rea-
E(r, t) = γ (r, t)mc2 . (11.212) sonable assumption for laser pulses of durations of
less than 1 ps and electron densities of n e ≤ 1022 cm−3 .
Due to the dependence of γ on the electron velocity It should be noted that in a relativistic plasma the
|ṙ| the energy will vary widely on the length scale of the plasma frequency ωp depends on γ and therefore on
laser wavelength and the time scale given by the laser the laser intensity. The dielectric constant becomes neg-
frequency. If one is not interested in the fast, mostly ative for electron densities where the plasma frequency
oscillatory motion of the electrons one may average over ωp exceeds the laser frequency ω. In the nonrelativistic
time, yielding: case (γ = 1) an critical electron density n crit is defined

through the condition ω2p = ω2 yielding [11.1998]
a2 (r)
γ (r) = 1 + 0 . (11.213) ε0 mω2
2 n crit = . (11.217)
e2
The slow spatial dependence indicated in a02 (r) may,
For electron densities n e > n crit the plasma is called
for example, be due to the intensity variation over the
dense while it is underdense for n e < n crit . In prac-
focus of the laser beam, which usually occurs over much
tical units the critical electron density is given by
larger length scales than a wavelength.
n crit = 1.1 × 1021 (1 µm/λ)2 cm−3 . With this definition
The spatial dependence of the time-averaged energy
the dielectric constant may be rewritten
gives rise to a force called the ponderomotive force ne
εr = 1 − (11.218)
Fp = −∇ E(r) = −mc2 ∇ γ (r) . (11.214) γ n crit
Lasers and Coherent Light Sources 11.13 Generation of Ultrahigh Light Intensities and Relativistic Laser–Matter Interaction 837

He-gas jet
»1019 –1020 cm–3
Electron diagnostics
Scintillating screen
e– Magnetic spectrometer
2ù probe pulse
variable delay

Part C 11.13
y

z, k
Laser pulse CCD
2 × 1019 W/cm2 x, E Shadow images
80 fs, f/2.2 2ù self emission
interferometry
Nozzle
0.7 mm, 10 Hz

Fig. 11.238 Experimental setup. The main pulse is focused to an intensity of a few 19 W/cm2 into a pulsed He-gas jet,
where a relativistic channel due to relativistic self-focusing is forming. By splitting and frequency doubling part of the
main pulse a probe pulse is generated. This probe pulse is used for imaging and observing the laser–plasma interaction
on a time scale determined by the probe pulse duration of ≈ 100 fs. The electrons that are accelerated in the relativistic
channel are characterized by magnetic spectroscopy and nuclear reactions

Electromagnetic radiation propagates in a medium Pcrit [11.1999].


where εr > 0 and is reflected from a medium with εr < 0.
8πε0 m 2 c5 n crit n crit
The condition for light propagation is therefore n e /γ < P > Pcrit = 2
= 17.4 GW .
n crit . e ne ne
(11.219)
The index of refraction of the plasma is given by

n = εr . In an underdense plasma n is real and the laser The dynamic equilibrium of defocusing because of
pulse propagates. But n is a complicated function of diffraction and self-focusing due to nonlinear effects
intensity for two reasons: leads to a guiding effect for the high-intensity laser
pulse in a plasma called relativistic channeling. This phe-
1. At the center of the propagating laser pulse the in- nomenon has been observed experimentally. A typical
tensity is high. Therefore the ponderomotive force experimental arrangement is shown in Fig. 11.238.
pushes the electrons away from the center and the A Ti:sapphire laser (λ = 800 nm) with a total
electron density in the center decreases, increasing power of 8 TW is focused to an intensity of about
the index of refraction. 2 × 1019 W/cm2 into a helium gas jet from a noz-
2. The remaining electrons in the center gain higher zle with a very well-characterized gas density profile
energies in the laser field than those sitting at the (Fig. 11.239).
edges of the laser beam. This increases γ further and Figure 11.239 shows the relativistic channel which
thus increases the index of refraction at the center of extends over a length of about 300 µm, corresponding to
the laser beam. about 15 Rayleigh lengths of the laser focusing optics.
At the onset of the channel the electron density amounts
This means that a relativistic laser pulse self- to 5 × 1019 cm−3 21
0 . The critical density is 1.7 × 10 cm
−3

modulates the index of refraction in such a way that at λ = 800 nm. Therefore the total laser power of 8 TW
self-focusing of the laser occurs. As in other self- exceeds the critical power of Pcrit ≈ 0.6 TW obtained
focusing phenomena known from nonlinear optics from (11.219) substantially and relativistic channeling
self-focusing is countered by diffraction and there- is expected and observed. In addition a probe pulse at
fore self-focusing depends on a critical power rather λ = 400 nm was used to measure the electron density in
than on intensity. A laser pulse interacting with the channel interferometrically (Fig. 11.238). The result
a fully ionized plasma will therefore undergo self- shown in Fig. 11.240 gives the electron density profile
focusing if its total power P exceeds the critical power across the channel at the onset of the channel. It is ap-
838 Part C Coherent and Incoherent Light Sources

Finally it should be noted that optics in the relativis-


Electron density ne (1019 cm–3)
tic regime is always nonlinear. The index of refraction
is always intensity dependent due to the ponderomo-
8 End of channel
tive force and the intensity dependence of the electron
mass.
Start of channel
6
Electron Acceleration
Part C 11.13

Since in the relativistic regime of laser–plasma inter-


4 action charged particles may be accelerated to high
energies, it has been recognized for some time that laser
plasmas are an ideal medium for high-field compact
2
274 µm accelerators. The plasma as an ionized medium may
sustain much higher fields than it is possible to generate
0 Nozzle
with conventional accelerator technology, where mater-
–1000 –500 0 500 1000
z-position (µm) ial breakdown imposes a limit at less than 100 MV/m.
Electric fields in the TV/m range may however be
Fig. 11.239 The lateral plasma density profile above the generated in laser plasmas.
nozzle has a Gaussian shape (dotted line). The density along In many experiments over the past two decades
the channel and its position is indicated by the bold line. a variety of acceleration mechanisms have been iden-
The inset shows the corresponding observed channel of the tified. A selection of these mechanisms will briefly
same spatial region. The extension of the emission indicates be described in the following with focus on schemes
a channel length of 274 µm, about 12 times the Rayleigh where only a single laser pulse is needed to acceler-
length of the laser. The relativistic channel starts near the ate initially resting electrons to relativistic energies. All
steepest density gradient and ends close to the maximum these schemes have in common that a laser pulse is fo-
density (grad n e = 0) cused into a gas jet, generating an underdense plasma
(Fig. 11.238).
parent that the electron density at the channel center is
depressed, due to the expulsion of electrons because of Laser wakefield acceleration. When a relativistic laser
the ponderomotive force. This result also provides di- pulse impinges on a plasma the ponderomotive force
rect evidence for the guiding structure of a relativistic expels electrons in both the transverse and longitudinal
channel. directions. The electrons expelled from the laser pulse
in the backward direction lead to a plasma wave called
the laser wakefield (Fig. 11.241) [11.2000].
The plasma wave follows the driving laser pulse with
ne/nc a phase velocity determined by the laser pulse group
velocity. The electric fields associated with the plasma
0.01
wave are now longitudinal. An electron can ride on the
0.005
plasma wave and be accelerated to relativistic energies in
the direction of laser propagation. This process is called
0 laser wakefield acceleration (LWFA).
50 This process is most efficient when the laser pulse
length cτ, where τ is the pulse duration, is shorter than
100
the plasma wavelength λp = 2πc/ωp .
150
50
0 This condition is depicted in Fig. 11.241a. When
150 100
z (µm) 200 250 200 a large number of electrons acquire a velocity close to
300 y (µm)
the phase velocity of the plasma wave, wave-breaking
Fig. 11.240 Plasma density at the start of the channel deter- occurs. The fast electrons are surfing on the wake of the
mined by interferometry. The electron density in the walls plasma wave.
of the channel rose up to values of n e (wall) = 6 × 1019 cm −3 .
The image in the upper right corner shows the interferogram Self-modulated laser wakefield acceleration. If the
from which the plasma density was obtained laser pulse length is longer than the plasma wavelength
Lasers and Coherent Light Sources 11.13 Generation of Ultrahigh Light Intensities and Relativistic Laser–Matter Interaction 839

cτ > λp the laser pulse undergoes a self-modulation


instability. The leading edge of the laser pulse drives a) ne , I b) I
a plasma wave. The electron density modulation of
the plasma wave in turn represents a periodic modu-
lation of the refractive index. It acts on the long laser
pulse such that the pulse is self-modulated and breaks
up into a train of short pulses (Fig. 11.241b). These

Part C 11.13
shorter pulses now match the conditions for LWFA
and can resonantly drive a plasma wave. This self-
z – ct z – ct
modulated laser wakefield acceleration (SM-LWFA)
is not as efficient as pure LWFA, but still high- Fig. 11.241 (a) LWFA: a short laser pulse (cτ ≤ p) shown as a dashed
energy even quasi-monoenergetic electron beams may line drives a plasma wave. (b) SM-LWFA: an initially long laser
be generated. pulse (dashed line) breaks up into a train of shorter pulses that
match the condition of LWFA and resonantly drive a plasma wave
Direct laser acceleration. Another acceleration pro- (after [11.1999])
cess which is quite different in nature to wakefield
acceleration is direct laser acceleration (DLA) which nal direction reaching TV/m is generated, which leads
is closely related to the formation of a relativistic to efficient electron acceleration.
channel. The ponderomotive force expels electrons
from the laser beam axis and generates a radial qua- Experiments. Numerous laser acceleration experiments
sistatic electric field. Electrons that are accelerated along have been carried out, mostly using experimental setups
the laser propagation generate an azimuthal magnetic like the one shown in Fig. 11.238. Initially always quasi-
field. The combination of these two fields results in exponential electron spectra were obtained with electron
an effective potential well for relativistic electrons. temperatures that follow the scaling law
Electrons trapped in this well will oscillate at the fre- ⎛ ⎞
 √ 2
quency ωβ = ωp / 2 γ , the betatron frequency. If a
kTe ≈ mc2 ⎝ 1 + 0 − 1⎠ , (11.220)
the trapped electron is moving fast enough along the 2
laser propagation, the laser oscillations may be in
phase with the betatron oscillations in the frame of the which corresponds to the kinetic energy of the elec-
electron. tron in the laser field. These exponential spectra
In this case, an efficient energy coupling is possible.
The energy gained by the electron in this process directly
Number of electrons per relative energy
results from the laser field and therefore the name direct spread per steradian [N/(dE/E) / Ù]
laser acceleration is appropriate.
3 × 1010

Bubble acceleration. A novel regime of laser wake- 2.5 × 1010


field acceleration, called bubble acceleration, was
proposed in 2002 on the basis of particle-in-cell 2 × 1010
(PIC) simulations [11.2002]. Short (τ < 7 fs) and in-
tense (a0 > 1) laser pulses were predicted to produce 1.5 × 1010
quasi-monoenergetic electrons with energies exceeding
100 MeV. 1 × 1010
The ponderomotive force also plays an important
role for this acceleration mechanism. In a frame mov- 5 × 1010
ing with an intensive laser pulse propagating through
a plasma the electrons are expelled from the center of the 0
20 40 60 80 100 120
pulse in both the longitudinal and transverse directions. Electron energy (MeV)
It turns out that behind the laser pulse an electron density
depression, called a bubble, is generated and electrons Fig. 11.242 Monoenergetic electron spectrum generated
the stream around this bubble and enter it again from the in an experimental setup similar to the one shown in
back side. In this way a strong electric field in longitudi- Fig. 11.232 [11.2001]
840 Part C Coherent and Incoherent Light Sources

are not only observed in underdense plasmas but gies by a mechanism quite different from the mechanism
also in the overdense plasmas encountered in laser– involved in electron acceleration.
solid interactions [11.2003]. For a typical intensity of As discussed earlier the interaction of an intense
I = 1020 W/cm2 and λ = 1 µm, a0 = 8.5 we obtain light field with matter yields the generation of a hot
kTe ≈ 2.6 MeV from (11.220). plasma and the subsequent acceleration of electrons
Only recently, however, has it became possible up to relativistic energies. Protons and ions are ac-
to generate monoenergetic electron spectra. As pre- celerated by a well-controlled mechanism known as
Part C 11.13

dicted by numerical simulations the bubble regime target normal sheath acceleration (TNSA) following
may be reached for high-power, gently focused laser the initial electron acceleration (Fig. 11.243). Fast elec-
pulses of short pulse duration. Although the require- trons are accelerated by an intense laser pulse (intensity
ments of the pure bubble regime have not yet quite I ≥ 1019 W/cm2 ) from the surface of a thin metal foil in
been reached experimentally the experiments show that the forward direction. They penetrate the foil and ion-
in the transition regime between LWFA and bubble ize atoms along their paths. Within about a picosecond,
acceleration monoenergetic electron spectra may be gen- those electrons leaving the target at the rear surface (that
erated [11.2001, 2004, 2005]. A typical result is shown is, the back surface with respect to the laser irradiation)
in Fig. 11.242. build up a quasistatic electric field. The field acts nor-
mally to the target surface, has cylindrical symmetry and
Ion Acceleration decreases in the transverse direction. Owing to the ultra-
Relativistic laser–matter interaction also leads to the short duration of the electron bunch and its high charge,
generation of monoenergetic beam of ions of MeV ener- this field may reach values of several TV/m close to
the axis and thus the potential can attain several tens of
MeV. Protons and positively charged ions present on the
Thin foil target with back surface of the foil may be accelerated by this field
polymer dot until they compensate the electron charge. In most cases,
20 × 20 × 0.5 µm3
the origin of these parasitic protons has been identified
to be a hydrocarbon contamination layer on the target
Laser incidence surface.
As the duration of the acceleration is ultrashort and
the protons (as well as the ions) are at rest before accel-
eration, comprising a very small phase-space volume,
the transverse emittance of the proton beam reaches val-
Hot electron ues as low as a few 10−3 mm mrad for 10 MeV protons.
Blow-off cloud However, laser-accelerated ion beams still show an en-
plasma ergy spectrum exhibiting a quasi-exponential shape with
a distinct cut-off energy. This can be explained by the
inhomogeneous distribution of electrons in the sheath,
Nd: YAG which causes an accelerating field that is inhomogeneous
ablation laser
in the transverse direction. For a plane and unstructured
target, the transverse dimension of the electric field and
hence the source size of the accelerated protons is much
Fig. 11.243 Laser acceleration of protons from the back side of a mi- larger than the laser’s focal spot. Therefore, different par-
crostructured target. A terawatt (TW) laser pulse is focused onto the asitic protons experience a range of potentials, resulting
front side of the target foil, where it generates a blow-off plasma in a broad distribution of energies.
and subsequently accelerates electrons. The electrons penetrate the Following this understanding of the mechanism of
foil, ionize hydrogen and other atoms at the back surface and set up laser acceleration of protons, it was pointed out that
a Debye sheath. The inhomogeneous distribution of the hot electron the resulting proton energy spectrum has a strong cor-
cloud causes a transversely inhomogeneous accelerating field [target relation to the spatial distribution of the protons on the
normal sheath acceleration (TNSA)]. Applying a small hydrogen- target surface. In order to generate high-quality proton
rich dot on the back surface enhances the proton yield in the central beams with monoenergetic features, a bilayered, mi-
part of the accelerating field, where it is nearly homogenous. These crostructured target, consisting of a thin high-Z metal
protons constitute the quasi-monoenergetic bunch foil and a small proton-rich dot on the back surface
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 841

was proposed. The transverse dimension of such dots is however at least two challenges laser accelerators that
smaller than that of the acceleration sheath, and hence have to overcome before widespread applications will
the protons will only be subject to the central – that become attractive.
is, homogeneous – part of the acceleration field. In In order to reach energies in the TeV range
this configuration, the protons all experience the same multistaging of both electron and ion accelerators
electric field and are accelerated in the same potential appears necessary. Although energy, beam quality
(Fig. 11.243). The resulting proton beam has a spectrum and charge per bunch are already attractive for

Part C 11.14
with a strong monoenergetic peak [11.2006]. low-energy applications of laser accelerators their av-
Recent experiments with a 10 TW, 600 mJ laser erage power presently remains orders of magnitude
showed that in this way quasi-monoenergetic proton below the average power of conventional acceler-
beams containing 108 protons with energies of a few ators. This is solely due to limitations in laser
MeV and a relative width of ∆E/E ≈ 10% and a total technology and may be overcome in the future
charge of about 100 pC were generated. when high-average-power high-intensity lasers become
In a different experiment quasi-monoenergetic car- available.
bon ions of 4 MeV energy were generated from a very Laser accelerators have already been used for
thin carbon layer on a metal target [11.2007]. a number of demonstration experiments. Low-energy
nuclear reactions have been induced using high-intensity
Applications and Future Developments lasers [11.1999] and nuclear transmutation scenarios
Relativistic optics leads to laser particle accelerators employing lasers have been discussed [11.2008]. Laser-
that are considerably more compact than classical ac- generated ion beams carry enough dose for radiation
celerators. Presently laser accelerators reach maximum therapy using ion beams, a very promising application
energies for monoenergetic electron beams approaching because the average power of a laser accelerator is al-
1 GeV and several MeV for monoenergetic ion beams ready sufficient for this innovative method of cancer
with a total charge of up to 1 nC per bunch. The scal- treatment.
ing for both electron and ion acceleration with laser and With ever-increasing laser intensities other areas
target parameters appears to be sufficiently well under- of physics such as gravitational physics, elementary
stood that electron energies exceeding 1 GeV and ion particle physics or nonlinear quantum electrodynamics
energies of a few hundred MeV in a single acceleration (QED) effects [11.1999] also come into the focus of
stage appear to be possible in the near future. There are high-intensity lasers.

11.14 Frequency Stabilization of Lasers


Soon after the development of the first HeNe laser, it was the general methods of laser frequency stabilization and
realized that the radiation of a continuous-wave laser to describe some representative examples of frequency-
would be ideally suited as a measurement tool, provided stabilized lasers. The radiations of a variety of stabilized
its frequency was stable and reproducible. Applications lasers are recommended as optical reference frequen-
of frequency-stabilized lasers include high-resolution cies [11.2009].
laser spectroscopy, quantum optics, optical frequency Basically, the frequency of any laser is determined
standards, the determination of fundamental constants, within the bandwidth of its amplifying medium by the
and the detection of gravitational waves. In these var- optical length of the resonator. This optical length in turn
ious cases, the requirements on frequency-stabilized is a function not only of its actual geometrical length
lasers are quite different. For example, optical frequency but also of the refractive index of the gain medium
standards and optical clocks need the smallest possi- itself, which may depend on several different param-
ble uncertainty in the knowledge of the absolute laser eters. The width of the gain profile may vary between
frequency whereas gravity-wave detectors need lasers a few 10−6 ν for gas lasers up to approximately 10% for,
of extremely low frequency noise while the absolute e.g., dye lasers or laser diodes. Different types of lasers
laser frequency is less important. Hence, different sta- have different noise characteristics. In most cases, the
bilization methods have been developed to address the dominant frequency noise is of technical nature and is
various tasks. The purpose of this chapter is to review far above the Schawlow–Townes limit [11.2010]. Since
842 Part C Coherent and Incoherent Light Sources

such technical frequency fluctuations are relatively slow of two lasers are coaxially combined by a beam splitter
they can be controlled by a suitable electronic servo sys- and focused onto a fast photodetector. The beat fre-
tem even if the frequency excursions of the free-running quency νB shows up as an oscillation in the power of the
laser are large. Different laser types and the specific combined laser beams. The photodetector transforms
requirements on these lasers have led to a variety of it to an oscillation of the photocurrent, provided νB is
stabilization methods. Within the limited space of this small enough that it can be processed by state-of-the-art
article, it is impossible to present a comprehensive and electronics.
Part C 11.14

detailed description of all these stabilization schemes. Frequency fluctuations of a laser can be measured
Hence, we concentrate on the description of the basic in both the frequency and time domain. Measurements
principles of laser frequency stabilization. For a deeper in the frequency domain are often used at higher fluc-
understanding, the reader is encouraged to study the ref- tuation (Fourier) frequencies whereas slower-frequency
erences given in this article as well as textbooks on laser fluctuations and drifts can be measured conveniently in
spectroscopy and optical clocks [11.2011–2014]. the time domain (see below).
We start with a brief discussion of the terms char-
acterizing the frequency behavior of a laser. These Spectral Density of Frequency Noise
are noise, stability, line width, reproducibility, and In the frequency domain, fluctuations δν at the fre-
the uncertainty of the laser frequency. Section 11.14.2 quency f can be detected by a frequency discriminator,
describes the basics of laser frequency stabilization. Ex- which converts frequency fluctuations to proportional
amples of stabilized lasers are presented in Sect. 11.14.3. voltage fluctuations. Since the noise components are not
Section 11.14.4 explains a universal method of opti- correlated, it is convenient to describe the fluctuations
cal frequency measurements by means of mode-locked δν( f ) by the mean square δν( f )2  which occurs within
femtosecond lasers. a bandwidth B at the Fourier frequency f . This value
is equivalent to the spectral noise power. The power
11.14.1 Characterization spectral density is then defined as Sf = δν2 /B and the
of Noise, Stability, Line Width, integration of Sf over B results in the total power of the
Reproducibility, and Uncertainty frequency noise within the bandwidth B. For the relative
of the Laser Frequency power spectral density S y we get S y = (δν/ν)2 /B.
To a good approximation, the frequency noise of
Noise, stability, line width, reproducibility, and the un- any oscillator can be modeled by a power series of the
certainty of the frequency are important parameters of Fourier frequency
any frequency-stabilized laser. In general, the laser fre-

2
quency fluctuates about a mean value which itself may Sy = cα f α . (11.221)
drift and walk randomly. Such variations may be caused, α=−2
e.g., by changes in the temperature, air pressure, vibra-
Depending on the exponent a the five terms of (11.221)
tions, acoustics or by fluctuations within the active laser
describe
medium itself.
The variations in the laser frequency can be investi- • a random frequency walk for α = −2
gated, e.g., by measuring the beat frequency νB = |ν1 − • flicker (1/ f ) frequency noise for α = −1
ν2 | between two identical but independently stabilized • white frequency noise for α = 0
lasers 1 and 2 (Fig. 11.244). For this purpose, the beams • flicker (1/ f ) phase noise for α = 1
• white phase noise for α = 2
Detector + Superimposed on the noise given in (11.221), we may
amplifier
also find peculiarities in the noise spectrum that are gen-
BS |í2 – í1| Frequency
Laser 1 erated by noise sources specific to the individual laser.
í1 í 1, í 2 counter
Such noise may be generated, e.g., by environmental
sources such as the excitation of mechanical resonances
Spectrum in the laser resonator, by instabilities of the mechani-
Laser 2
í2 anaylzer cal setup, or by fluctuations in the refractive index of
the laser medium. Furthermore, the laser frequency is
Fig. 11.244 Schematics of a beat-frequency measurement sensitive to optical feedback and careful isolation of the
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 843

laser system from back-scattered light is important for νn+1 in (11.222)


successful operation of stabilized lasers. Usually, the

(n+1)τ
different noise components show up at different Fourier 1
frequencies. Hence, the detection of these noise compo- νn+1 = νi (t) dt (11.223)
τ
nents helps us to identify the various noise sources and i=nτ
to reduce their influence. In addition, the knowledge of represent the mean frequency averaged during the n-th
the frequency noise spectrum of a free-running laser is interval of duration τ. Since it is difficult to measure

Part C 11.14
also important for the design and optimization of the the optical frequency directly, it can be down-converted
frequency control system. by beating the laser radiation against the radiation of
The noise spectra of various types of lasers may a second laser such that the beat frequency arrives in the
be quite different. For example, most of the frequency radio-frequency range, where it can be counted directly.
noise in gas lasers such as HeNe or CO2 lasers oc- In this case, the measurement contains the instabilities
curs at low Fourier frequencies. It is generated in part of both lasers. If the two lasers are identical but indepen-
by mechanical instabilities of the laser setup. The cor- dent, we can assume that both lasers contribute equally
responding frequency excursions δν may amount to to the standard deviation √ and consequently, the meas-
a few MHz at Fourier frequencies up to about 10 kHz. ured value corresponds to 2 times the Allan deviation
In addition, random-walk and flicker (1/ f ) frequency σ y (τ) of a single laser.
noise shows up at these low frequencies. Neglecting The dependence of σ y (τ) on the averaging time τ
further possible noise sources originating from plasma contains information about the frequency noise spectrum
resonances of the discharge, the noise spectrum at of the laser. If the relative power spectral density of
higher Fourier frequencies may be approximated by the noise S y is known, σ y (τ) can be calculated by the
white frequency noise. In tunable CW dye lasers, on relation [11.2016]
the other hand, the frequency noise is much larger
∞
than in gas lasers. It is generated mostly by variations (sin π f τ)4
in the thickness and the refractive index of the dye σ y2 (τ) = Sy ( f ) df . (11.224)
(π f τ)2
jet, which is flowing at high speed through the small 0
active volume of the laser. Hence, rather strong fre-
For the different models of the noise process given in
quency fluctuations are observed at Fourier frequencies
(11.221), we can describe the Allan variance σ y2 (τ) by
around 50 kHz. At higher Fourier frequencies the influ-
the relation
ence of the dye jet decreases and hence the noise also
decreases, eventually reaching the photon shot-noise σ y2 (τ) = dα τ β (11.225)
level.
where β is determined by the relation [11.2016]

Allan Standard Deviation ⎨−α − 1 for α ≤ 1
Slow variations, in particular drifts and random walk of β= (11.226)
the laser frequency can be measured conveniently in the ⎩−2 for α > 1
time domain by counting the mean frequency ν within
a time interval τ. Such measurements are advantageous and dα is a constant. The dependence of σ y2 (τ) on τ is
if changes in the frequency within time intervals between listed for the noise processes of (11.226) in Table 11.55.
seconds and several hours are of interest. The relative Of course, any frequency modulation will also show
frequency instability in the time domain is characterized up in the Allan standard deviation. In the case that the
by the Allan deviation [11.2015, 2016]
Table 11.55 Dependence of the Allan deviation on τ for the
 1/2 different noise processes discussed in (11.226)
1 1 
N−1
σ y (τ) = (νn+1 − νn )2 , Noise category α β σ y2 (2, τ)
ν 2(N − 1)
n=1
White frequency noise 0 −1 ∝ 1/τ
(11.222)
White phase noise 2 −2 ∝ 1/τ 2
1/ f (frequency noise) −1 0 constant
where the root mean square of the difference between
1/ f (phase noise) 1 −2 ∝ 1/τ 2
two consecutive frequency measurements (νn+1 − νn ) is
used as a measure of the stability. The frequency values Random frequency noise −2 1 ∝τ
844 Part C Coherent and Incoherent Light Sources

gate time τ is an integer multiple of the modulation pe- determined by the size and spectral extension of these
riod τm = 1/ f m , where f m is the modulation frequency, sidebands. In the case of pure harmonic phase modu-
the influence of the modulation is eliminated. It will be lation, the field E of the laser radiation is given by the
maximum for τm = (2n + 1)/(2 f m ). With increasing in- relation
tegration times τ, the influence of the modulation washes
out and can be neglected, eventually. E(t) = E sin [Ω0 t + δφ sin (ωt)]

As a result of (11.227), we find that the noise pro-
= E J0 (δφ) sin(Ω0 t)
Part C 11.14

cess can be estimated from the slope of a log–log σ y (τ)


plot. For example, in a HeNe laser that is frequency sta- ∞

bilized to an absorption line of molecular iodine, σ y (τ) + Jn (δφ) exp[i(Ω0 + nω)t]
decreases in a wide range of τ with the square root of n=1
τ corresponding to a slope of −1/2, (Fig. 11.245) indi- ∞ 
cating white frequency noise within the corresponding + Jn (−δφ) exp[i(Ω0 − nω)t] ,
time interval τ. At longer integration times, σ y (τ) flat- n=1
tens out due to flicker frequency noise and in some cases (11.227)
eventually increases again due to drifts and random fre-
quency walks. For practical applications, the σ y (τ) plot where Ω0 = 2πν0 and ω = 2π f represent the carrier and
indicates the minimum integration time τ necessary to modulation frequency, respectively; δφ = δν/ f is the
achieve a given statistical frequency uncertainty. modulation index with δν the amplitude of the frequency
deviation. The amplitude of the n-th sideband given by
Line Width of Laser Radiation the n-th order of the Bessel function Jn (δφ) decreases
In incoherent light sources such as spectral lamps, where strongly with n for n > δφ. Basically, we can distinguish
the radiation consists of uncorrelated photons emitted between the two limiting cases of
within a certain narrow frequency band, the line width is 1. large frequency fluctuations δν at low Fourier fre-
determined by a superposition of the natural width of the quencies f and
transition and Doppler broadening. It can be measured, 2. small, fast frequency fluctuations δ f in a broad band.
for example, by a high-resolution scanning Fabry–Pérot
interferometer. In the case of laser radiation, the line Case 1 is frequently observed with laser resonators,
broadening is caused by frequency fluctuations of the which pick up environmental acoustic or mechanical
continuously emitted coherent laser radiation. The fre- noise. The mean amplitudes δν2 1/2 of such fluctua-
quency fluctuations generate noise sidebands that cause tions may be in the range between a few 10 kHz up to
broadening of the laser spectrum. The line width is then several megahertz, whereas they usually occur at Fourier
frequencies in a range below 1 kHz. Hence the modula-
tion index δϕ 1. In this case, the line width is given
ó (ô) by [11.2017]
10–10  1/2
∆νFWHM = 8 ln (2)δν2 

= 2.355δν2 1/2 (11.228)
ô –1/2

10–11 close to the frequency excursions between the peaks.


If the servo gain of the frequency stabilization is
high enough to reduce the frequency fluctuations at
low Fourier frequencies, we may observe case 2. Un-
der the assumption that we can neglect frequency drifts
10–12 and frequency changes at very low Fourier frequencies,
we arrive at frequency fluctuations (δν2 )1/2  B and
correspondingly to a small modulation index. In this
1 10 100 1000 case, only the amplitudes of the first-order sidebands
ô (s)
Jn (δφ) and J−n (δφ) contribute significantly to the line
Fig. 11.245 Allan deviation σ y (τ) versus integration time τ width. If the spectral density Sf is constant, the line
of an iodine-stabilized HeNe laser profile is Lorentzian and the line width is given by the
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 845

relation [11.2017] signal-to-noise ratio, allowing a fast servo lock. How-


ever, since the laser frequency is coupled to the length of
∆νFWHM = π Sf . (11.229)
an artifact, it may change in time. Stabilization to such
artifacts is often applied as an intermediate step to re-
Frequency Reproducibility and Uncertainty duce the line width of the laser emission and to allow for
of Laser Radiation high spectral resolution. In a second step, the frequency
Whenever the laser frequency is needed as a precise ref- can then be stabilized to an absolute frequency reference

Part C 11.14
erence, knowledge of the reproducibility and uncertainty provided by a suitable atomic or molecular absorption
is essential. Since the frequency of the stabilized laser line.
depends on various operational and environmental pa- The following sections give an introduction to ba-
rameters it is necessary to analyze this dependence and sic methods of laser frequency stabilization. We start
to control these parameters carefully. The frequency re- with the generation of the error signal and review four
producibility is a measure of the scatter in the frequency prominent examples. The first two methods – the side-
values either of an ensemble of differently designed of-the-fringe stabilization and the phase-modulation
laser systems of the same kind, developed for exam- (Pound–Drever–Hall) technique are used to stabilize the
ple in different laboratories. The reproducibility can then laser frequency to a resonance of a stable optical cavity.
be investigated by frequency inter-comparisons between Absolute frequency stabilization to an atomic reference
such differently designed lasers. Alternatively, the term is then reviewed and the fundamentals of the electronic
frequency reproducibility is also used to describe the servo-control system are described.
scatter in the frequency of a single laser caused by the
uncertainty in the precise control and optimization of Generation of the Error Signal
the operation parameters. Basically, the frequency stabilization of a laser converts
The frequency uncertainty is a measure of how ac- the frequency deviation δν = νl − ν0 between the laser
curately we can realize the reference frequency and frequency νl and the reference frequency ν0 to an error
determine its value. Basically, the total uncertainty signal that is proportional to δν. This signal is amplified
contains two contributions. The first represents the by a servo amplifier and used to control the laser fre-
uncertainty to which the transition frequency of an un- quency such that the error signal vanishes. Figure 11.246
perturbed atomic or molecular absorber at rest can be shows the basic scheme of a stabilization to an atomic
realized. This part contains all values in the uncertainty reference frequency.
of frequency shifts caused by environmental and/or op-
erational conditions. Such shifts may be generated, e.g., Side-of-the-fringe stabilization. In commercial sta-
by a residual Doppler effect, by collisions, and by ex- bilized lasers such as tunable dye lasers, it is
ternal fields. The second term in the total uncertainty is a well-established practice to stabilize the frequency to
linked to the determination of the frequency value. Such a resonance of a stable optical cavity. The frequency
frequency measurements have to be referenced to the
primary standard of time and frequency, the Cs atomic
clock. If the frequency measurement is phase-coherent, Atoms, molecules, or ions
the measurement itself does not contribute to the total
uncertainty. Under this condition, the uncertainty of the Laser Detector
optical frequency is determined only by the uncertainty
of the standard itself and that of the Cs reference. s
í0
í0 í
11.14.2 Basics
of Laser Frequency Stabilization Electronic Absorption
servo control signal
In any active frequency control system, the laser fre-
quency is servo-controlled to a reference frequency. This
may be provided by an eigenfrequency of a stable optical í
Error signal í0
(Fabry–Pérot) resonator, by the gain profile of the laser
itself, or by a suitable atomic or molecular transition. Fig. 11.246 Schematic of a laser frequency stabilization to
The first case has the advantage that it provides a good the center of an absorption line
846 Part C Coherent and Incoherent Light Sources

discriminator is provided by the side of a transmission the speed of the servo control is ultimately limited by
fringe [11.2018]. The basic idea is that the sloping side the response time of the cavity [11.2019]. Furthermore,
of the fringe converts the laser frequency fluctuations to the locking range of the servo control is asymmetric.
amplitude fluctuations with high conversion efficiency For example, if the laser frequency is locked to point A
and a good signal-to-noise ratio. To prevent laser ampli- (Fig. 11.247b), the locking range towards lower frequen-
tude noise from entering the discriminator channel, two cies corresponds almost to the total free spectral range of
balanced photodetectors are used (Fig. 11.247a). One the cavity, whereas for higher frequencies it corresponds
Part C 11.14

looks at the frequency-selective transmission of the res- only to approximately one full width at half-maximum.
onator and the other views an attenuated portion of the Hence, spontaneous and fast excursions towards higher
input beam. frequencies exceeding the half-width may force the laser
The attenuation is adjusted such that the resulting to fall out of lock and relock at the next-higher interfer-
difference of the two photodetector signals crosses zero ence order. To increase the locking range and to avoid
at the half-point of the maximum transmission. In a fre- such unwanted frequency jumps, commercial lasers usu-
quency interval close to the zero crossing, the signal ally apply reference resonators of rather low finesse
depends almost linearly on the frequency deviation δν at the cost of a strongly reduced sensitivity. Neverthe-
and can be used as an error signal for stabilization. This less, side-of-the-fringe stabilization has been used very
side-of-the-fringe method is quite simple and very useful successfully in many stabilized lasers.
for many applications. However, if high spectral reso-
lution and low drift rates are required, it turns out that Phase-modulation technique. Many of the shortcom-
the reference frequency is not defined precisely enough. ings of the side-of-the-fringe method are avoided if the
For example, if the direction of the laser beam inci- laser frequency is locked to the center of a symmetric
dent to the resonator changes, the transmission will also resonance. This can be achieved in transmission or re-
change whereas the power in the other reference beam flection. In the latter case, the amplitude of the return
stays constant. Hence, the zero crossing of the error sig- beam is a superposition of the beam reflected directly at
nal changes, leading to a shift of the stabilized laser the entrance mirror and a small part of the light stored
frequency. A further difficulty arises from the fact that inside, which is leaking out of the cavity. At resonance,
the two beams interfere destructively and the intensity
of the return beam has a minimum at the line center.
a) Reference It follows that an abrupt change of the laser frequency
resonator shows up instantaneously in the interference signal be-
BS PD 1
tween these two beams and the transient behavior of the
resonator does not limit the bandwidth of the servo con-
trol [11.2020, 2021]. Hence, a servo bandwidth up to
a few megahertz can be achieved even with ultrahigh-
PD 2
finesse cavities with line widths in the low kilohertz
range.
Variable attenuator Fast stabilization techniques to line center have been
S developed [11.2022–2024] utilizing either DC or radio-
b) frequency (RF) methods. In the following, we describe
an RF method where the signal is detected in reflection.
This method was introduced by Pound [11.2025] to sta-
A B bilize the frequency of a microwave oscillator and later
í applied in the optical range by Drever (the PDH tech-
nique) [11.2023]. To generate the error signal, the phase
of the laser radiation is modulated at a radio frequency.
For an optimum signal size, the modulation frequency
should be larger than the width of the cavity resonance.
í0
A high modulation frequency is also advantageous, since
Fig. 11.247a,b Frequency stabilization to the side of the influence of 1/ f noise decreases and can eventually
a fringe. (a) Experimental setup, (b) either point A or point B be neglected, leading to a signal-to-noise level close to
can be selected as the reference the shot-noise limit.
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 847

The basic experimental setup of the PDH stabiliza-


tion scheme is shown in Fig. 11.248. A small fraction of a) Signal
the laser power (< 10%) is split off the main laser beam
ö=0
and used for the stabilization. It is phase modulated by
an electrooptic modulator (EOM). The modulation fre-
quency (typically ≈ 15 MHz) is several times larger than
the width of the resonance. The modulation index δν/ f m G=1 =3 =5 =7 =9

Part C 11.14
is in the range 10–30%. After passing a polarizing beam
–6 –4 –2 2 4 6
splitter (PBS) and a 45◦ Faraday polarization rotator
(FR), the incident beam is mode-matched into the refer-
(í – í0) / íh
ence resonator. The polarization of the returning beam
is rotated by another 45◦ . Hence, the incident and the re-
turning beam are polarized perpendicular to each other
and separated by the PBS. The return beam is sent to b) Signal
a photodetector (PD).
ö = ð/2
If the laser frequency is tuned far from resonance,
the carrier and the sidebands of the modulated beam
are promptly reflected and no intensity modulation is G=1 =3 =5 =7 =9
observed by the photodetector. If the carrier or either
sideband approaches the cavity resonance, its ampli- –6 –4 –2 2 4 6
tude and phase changes depending on the detuning of (í – í0) / íh
the corresponding frequency component from the cav-
ity resonance. The other frequency components which
are off-resonance are promptly reflected. Hence, in the
returning beam, the balance between the carrier and the
sidebands is broken and power modulation is gener- Fig. 11.249a,b Demodulated signals versus detuning ob-
ated. The corresponding amplitude modulation of the served with the PDH technique, (a) in phase (ϕ = 0)
photocurrent is phase-sensitively detected by the PD fol- and (b) in quadrature (ϕ = π/2) with the modulation.
lowed by a double-balanced mixer, which is driven at the G = (νm /νh ) corresponds to the ratio between the modula-
modulation frequency. The corresponding demodulated tion frequency νm and the half-width νh of the resonance
signals – after passing a low-pass filter – are shown
for different modulation frequencies G versus the laser
frequency in Fig. 11.249a in phase and Fig. 11.249b in
quadrature with the modulation voltage at the EOM.
To experiment Reference
Isolator resonator In the first case (Fig. 11.249a), we observe a disper-
EOM PBS sive signal D(∆) with zero crossings at the resonance of
BS
the carrier and close to the resonances of the sidebands.
Isolator PD
It is given by the relation [11.2013].
rf
D(∆)
Ω 2 Γ∆(Γ 2 + Ω 2 − ∆2 )
Laser ∝ .
DBM (∆2 + Γ 2 )[(∆ + Ω)2 + Γ 2 ][(∆ − Ω)2 + Γ 2 ]
(11.230a)
The absorptive signal A(∆) (Fig. 11.249b) is given by
Servo amplifier A(∆)
ΩΓ∆(Γ 2 + Ω 2 + ∆2 )
Fig. 11.248 Schematic of the PDH frequency stabilization ∝ .
technique (see text) (BS: beam splitter, PBS: polariz- (∆2 + Γ 2 )[(∆ + Ω)2 + Γ 2 ][(∆ − Ω)2 + Γ 2 ]
ing beam splitter, EOM: electrooptic modulator, RF: (11.230b)
modulation-frequency generator, PD: photodetector, DBM: In (11.230), Γ /2π = νh is the half-width at half-
double balanced mixer) maximum of the cavity resonance, Ω/2π is the
848 Part C Coherent and Incoherent Light Sources

modulation frequency, and ∆/2π = (ν − ν0 ) is the fre- the laser can be estimated only by methods independent
quency detuning. of the actual servo loop, e.g., by beat-frequency com-
The central zero crossing of the dispersion signal parisons with a second laser or by the use of a second
D(∆) (Fig. 11.249a) is used as the error signal for the independent frequency discriminator.
frequency control. The signal detected in quadrature To achieve a narrow line width, it is important to
(Fig. 11.249b) shows a resonance feature when either isolate the cavity from any distortions, e.g., from vibra-
of the sidebands coincides with the cavity resonance. tions, acoustics, and temperature changes, caused by the
Part C 11.14

The different polarities of the two features are caused by environment. For this reason, the resonator is frequently
the phase difference π between the carrier and the up- vibration isolated and supported in a temperature-
per sideband and that between the carrier and the lower controlled vacuum chamber [11.2020, 2026]. A further
sideband. Independent of the detection phase, the de- cause of possible frequency offsets is a spurious resid-
modulated signal is always antisymmetric with respect ual amplitude modulation (RAM) of the intrinsic laser
to the central zero crossing. Consequently, a small phase beam. Such RAM may be generated, e.g., by an im-
deviation from zero does not change the frequency of the perfect phase modulator itself. Very often, RAM is also
central zero crossing. However, it will slightly change introduced by spurious interferences in the optical setup
the slope of the frequency discriminator and thereby the caused, for example, by light backscattered at the sur-
gain of the servo loop. faces of optical elements. The servo cannot distinguish
Since the returning beam results from an interference between the true error signal and the RAM. Hence, the
between the frequency components promptly reflected total of the superimposed signals are servo controlled to
at the entrance mirror and part of the stored radiation zero, leading to a nonzero error signal and consequently
leaking out of the cavity, any fast frequency change to a frequency shift. Usually, this spurious RAM varies
shows up as a change in the interference signal instanta- with time and we experience frequency fluctuations that
neously even if the response time of the cavity is much are not identified by the error signal of the servo loop.
longer. At low Fourier frequencies f , smaller than the At high spectral resolution, these fluctuations may be or-
half-width Γ /2π(2π f  Γ ), the transient response of ders of magnitude larger than those estimated from the
the cavity can be neglected and the demodulated sig- noise in the error signal. Hence, it is important to iso-
nal acts as a frequency discriminator. With increasing late the cavity from environmental disturbances and to
Fourier frequency, the signal turns to a phase discrimi- minimize the RAM very carefully.
nator for 2π f Γ . Hence, the amplitude A( f ) and the The narrowest line width achieved with the PDH
phase φ( f ) of the error signal, have a low-pass charac- method in a dye laser was as low as 0.5 Hz [11.2027]
teristic which rolls off with 1/ f for frequencies f above and even with diode lasers a line width in the range of ap-
the cut-off frequency Γ /2π [11.2020] proximately 1 Hz could be achieved [11.2021]. The PDH
stabilization technique is now used almost exclusively, if
1
A( f ) = A(0)  , a precision stabilization to a cavity resonance is required
1 + (2π f/Γ )2 combined with extremely high spectral resolution.
ϕ( f ) = − arctan(2π f/Γ ) . (11.231)
Stabilization to a Doppler-free atomic reference. The
If this integrating behavior for Γ > 2π f is taken into stabilization methods discussed above describe methods
account in the design of the servo amplifier, a servo to stabilize the laser frequency to a reference provided
bandwidth much larger than Γ /2π can be envisaged. Ba- by the length of an artifact. An absolute stabilization
sically, the servo bandwidth is limited to a few megahertz requires that the frequency is traced back to a natu-
by delays in the servo system. ral constant, e.g., to the center of a suitable atomic
If the frequency of the laser is stabilized, the size or molecular absorption line. Ideally, the frequency
of the residual error signal provides us with information of such transition should not depend on environmen-
about the quality of the servo electronics. However, this tal or operational parameters such as external fields,
error signal is by no means a measure of the actually atomic collisions, laser power, etc. The atomic reference
achieved frequency stability or laser line width. There line should be narrow and provide us with a sufficient
are still frequency fluctuations that are not detected by signal-to-noise ratio. The atoms may be contained in an
the electronic servo. In particular, at very high spectral absorption cell, in an atomic beam or stored in a trap.
resolution, small variations of the optical length in the At room temperature, the thermal velocity distribution
cavity can no longer be neglected. The true line width of of the atomic absorbers cause a Doppler broadening of
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 849

the line which is in the range of δν/ν ∼


= 10−6 and which
is usually much larger than the natural line width of the a) I (í) b) I 2 – I1
reference transition. An atom moving with a velocity I1
component vz in the direction of the laser beam sees I2
a Doppler-shifted frequency
 
νD = νl 1 ± νz /c + ν2 /(2c2 ) , (11.232) –2 –1 0 1 2 –2 –1 1 2

Part C 11.14
(í – í0) / íh (í – í0) / íh
where νl is the laser frequency and νz is the velocity com-
ponent in the direction of the laser beam. In (11.232),
the term νl νz /c represents the first-order Doppler effect.
The positive sign is valid for atoms counter-propagating Fig. 11.250 Generation of the error signal by a square-wave fre-
to the laser beam whereas the minus sign belongs to the quency modulation
co-propagating ones. The third term νl ν2 /(2c2 ) corre-
sponds to the (relativistic) second-order Doppler effect. inside, a Doppler-free feature caused by saturated ab-
Whereas the first-order Doppler effect can be strongly sorption will show up as a small symmetric dip in the
suppressed by the application of nonlinear Doppler- tuning curve of the laser at the center of the reference
free spectroscopic methods such as, e.g., saturated transition. This feature has to be converted to an error
absorption [11.2028, 2029] or Doppler-free two-photon signal which is antisymmetric with respect to the de-
excitation [11.2030, 2031] the second-order effect can tuning ∆ν = νl − ν0 . A simple concept to generate the
be reduced only by cooling the absorbers. error signal is to switch the laser frequency between
As a typical example of Doppler-free spectroscopy, two discrete values (Fig. 11.250a). The difference in the
we concentrate on the saturated absorption and give corresponding two absorption signals I2 − I1 leads to an
a brief description of this method. For simplicity, we antisymmetric error signal with a zero crossing at the line
neglect the influence of the second order Doppler effect. center (Fig. 11.250b). For small modulation amplitudes,
Let us consider an atomic ensemble which is excited by the error signal is proportional to the first derivative of
two counter-propagating laser beams of the same fre- the absorption signal.
quency νl . If νl does not coincide with the line center Instead of a square-wave modulation, most lasers
ν0 of the transition, the two beams will excite and sat- use a harmonic frequency modulation. Consequently,
urate two groups of atoms with velocity components νz the laser power will contain harmonics of the modu-
and −νz , of which the Doppler-shifted frequencies νD lation frequency. The amplitudes of these harmonics
coincide with the laser frequency νl . Consequently, two depend on the modulation width and on the detuning.
saturation holes are burned into the velocity distribution The amplitude of a particular harmonic signal in the
of the ground state. If we tune the laser frequency closer laser power can be detected by a photodetector followed
to the center of the line, |νz | decreases and the holes ap- by a phase-sensitive detector which is gated by the cor-
proach each other until they overlap for νz = 0 when the responding harmonic of the modulation frequency. For
laser frequency is tuned to line center. In this singular a symmetric absorption line, the amplitudes of the odd
case, the number of atoms contributing to the absorp- harmonics are antisymmetric and have a zero crossing
tion decreases and hence less laser power is absorbed, at ∆ν = 0. Hence, these odd harmonics are suitable as
resulting in a narrow Doppler-free absorption dip which error signals for frequency stabilization. In many cases,
is used as a reference for the stabilization. Hence, (first- third-harmonic detection is applied in order to suppress
order) Doppler broadening is suppressed and the width a residual slope [11.2032,2033]. If the modulation width
of this dip is determined by the natural width of the tran- is small compared to the line width, the derived signal
sition, by power and collision broadening of the line, and represents the corresponding derivative of the saturation
ultimately by the limited interaction time of the atoms signal, e.g., the first derivative for the first harmonic and
moving across the laser beam. To first order, the pro- the third derivative for the third harmonic.
file of this dip can be approximated by a Lorentzian line If we approximate the Doppler-free saturation fea-
shape. ture by a Lorentzian line profile I(ν).
As a practical example, let us consider an absorbing A
gas contained in a cell at low pressure. It can be placed I(ν) =  2 (11.233)
inside or outside the laser cavity. If the cell is placed 1 + (ν − ν0 ) /ν1/2
850 Part C Coherent and Incoherent Light Sources

we can estimate the amplitudes of the harmonics versus


the detuning for various modulation widths [11.2034]. a) A1 dD
0 2 4 6 8 10
In (11.233), A and ν1/2 are the height and the half-width 0.2
(HWHM) of the saturated absorption feature, respec-
tively. The modulated laser frequency ν(t) can be written –0.1
as
–0.2
ν(t) = ν0 + ∆ν + δν A cos(ωt) ,
Part C 11.14

(11.234)
–0.3
where ∆ν is the detuning of the mean laser frequency
from the line center ν0 and δνA is the modulation am- –0.4
plitude. If the modulation frequency ω/2π is small
compared to the line width, the detected signal follows –0.5
the laser frequency ν(t) closely and we can replace ν in
(11.233) by ν(t) of (11.234), leading to a time-dependent b) A3
absorption signal 0.2
A
I(t) = ' (2 .
1 + [∆ν + δνA cos(ωt)] /ν1/2 0.1

If we relate ∆ν and δνA to the half-width (HWHM) ν1/2


we get with the reduced detuning dD = ∆ν/ν1/2 and the 0
reduced modulation amplitude dA = δνA /ν1/2
–0.1
A
I(t) = . (11.235)
1 + [dD + dA cos(ωt)]2
0 2 4 6 8 10
The signal I(t) is periodic in time and can be expressed dD
by a Fourier series
Fig. 11.251 Amplitudes of the first harmonic ( A1 )

 and the third harmonic ( A3 ) versus the detuning
A0
I(t) = + Am cos(mωt) , (11.236) dD = ∆ν/ν1/2 . The modulation amplitude was cho-
2
m=1 sen as dA = 0.2, 0.6, 1.0, . . . , 3.0 for A1 , and dA =
where the Fourier coefficient Am represents the sig- 0.5, 1.0, 1.5, . . . , 6.0 for A3
nal amplitude of the m-th harmonic of the modulation
frequency ω/(2π). It can be calculated by the relation A1 and A3 are shown versus the detuning dD for
π various modulation amplitudes dA in Fig. 11.251a and
2 Fig. 11.251b, respectively. Both curves have zero cross-
Am = I(τ) cos(mτ) dτ .
π ings at dD = 0. In the central part, their amplitudes
0 depend linearly on the detuning dD . Hence, both sig-
For the coefficients A1 and A3 we get [11.2034] nals A1 and A3 can be used as discriminator signals for
frequency control. Their slope depends on the modula-
1  
A1 = (sign dD ) P− − dD P+ (11.237a) tion width dA . For small amplitudes dA  1, the slope of
dA the first-harmonic signal depends linearly on dA and that
and of the third harmonic increases with the third power of
1 ) 
 dA . The largest slope and consequently the highest sen-
A3 = 3
(sign dD ) 4 1 − 3dD
2
+ 3dA
2
P− sitivity can be obtained with the first harmonic A1 (dD ).
dA

 * In many cases, however, the saturation signal I(dD )
+ 4 3 − dD 2
+ 3dA
2
dD P+ − 16dD is superimposed on a frequency-dependent (sloping)
background. Consequently, a signal is added to the first-
(11.237b) harmonic signal A1 (dD ) and the zero crossing is shifted,
√  leading to a frequency offset of the stabilized laser fre-
with P± = ρ1 2(ρ ± α) and ρ = α2 + 4dD
2 and α =
quency. This shift can be strongly reduced if the third or
1 + dA
2 − d2 .
D a higher odd harmonic is applied for the stabilization.
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 851

A typical example of a laser utilizing the third-harmonic the servo gain should be as high as possible. In par-
detection technique is the iodine-stabilized HeNe laser ticular, the deviation of the mean frequency averaged
(see Sect. 11.14.3). over long times should be close to zero. This requires
that g( f → 0) → ∞. In any servo-control system, phase
Servo Amplifier and Filter shifts and time delays of the servo loop put limitations
This subsection describes how the error signal is used on the maximum gain and the bandwidth of the servo-
to control the laser frequency. If the servo control is op- control. A simple technique to provide high servo gain

Part C 11.14
erating, the initial frequency νi of the free-running laser at low frequencies and to reduce the influence of phase
is corrected by the servo loop to νS , which is close to shifts and time delays at high frequencies is to reduce
the reference frequency ν0 (Fig. 11.252). The difference the servo gain with increasing Fourier frequency f . Such
δν = νS − ν0 represents the residual frequency devia- a characteristic can be obtained by an integrating behav-
tion from the line center ν0 of the stabilized laser. The ior of the servo gain, i. e., if C Dg( f ) decreases with 1/ f
deviation δν is converted to an amplitude U = Cδν by for increasing frequencies. In this case, the total transfer
the error signal, where the constant C is proportional to function of the control system can be characterized by
the sensitivity of the frequency discriminator. The sig- a unity-gain frequency f C , the frequency at which the
nal Cδν is amplified in the following servo amplifier gain of the open servo loop C Dg( f C ) = 1. At low fluc-
by a factor g( f ) and is then transferred to a frequency tuation frequencies f  f C , the frequency deviations
transducer, which corrects the laser frequency νi by ∆ν( f ) will be reduced by a factor of f/ f C and an in-
−C Dg( f )δν. Here D is the sensitivity of the transducer, crease of the servo gain corresponds to a proportional
which transforms the control voltage to a corresponding increase of the unity-gain frequency f C . Consequently,
frequency shift of the laser. The term g( f ) characterizes in an integrating servo loop a high servo gain requires
the frequency-dependent gain of the electronic servo am- a large servo bandwidth f C . In cases where the servo
plifier. The servo loop provides a negative feedback to bandwidth f C is limited and where large frequency
the laser frequency and the corrected value νS can be fluctuations at low frequencies have to be suppressed,
written as an additional integration can be introduced, leading
to a double integrating behavior and consequently to
νS = νi − C Dg( f )δν (11.238)
a higher servo gain at low frequencies. The stability of
which can be transformed to the servo loop requires that this double integration is
δν 1
= , (11.239)
∆ν 1 + C Dg( f ) Servo gain
where ∆ν = νi − ν0 is the initial frequency offset of the
free-running laser. 106
–40 dB/decade
We see that the servo-control circuit reduces the
frequency deviation ∆ν of the free-running laser by
a factor of 1/[1 + C Dg( f )], where C Dg( f ) represents –20 dB/decade
104
the gain of the open servo loop. To achieve a negligi-
bly small value of the residual frequency deviation δν,
fdi
Unity
102 Cavity response gain
of PDH signal frequency
D g( f )
Response of
C D g (íS – í0) C (íS – í0) servo amplifier
100
íi C
íS (íS – í0) 0
100 Hz 10kHz 1 MHz
Frequency
í0
Fig. 11.253 Typical servo gain versus Fourier frequency of
Fig. 11.252 Equivalent circuit of a laser frequency stabiliza- a PDH frequency stabilization to a cavity resonance (see
tion text)
852 Part C Coherent and Incoherent Light Sources

effective only at frequencies well below the unity-gain two-photon excitation. Ultimately any frequency shifts
frequency f C . In practice, the maximum crossover fre- caused by a residual Doppler effect can be strongly re-
quency f di between single and double integration should duced if the laser radiation interacts with cold atomic
be smaller than f C /4. Figure 11.253 shows a typical de- absorbers only.
pendence of servo gain on the fluctuation frequency of This section is organized as follows. In the first part,
a frequency stabilization to a narrow cavity resonance we explain as a typical example the stabilization of a tun-
using the PHD technique. able diode laser to the resonance of a stable optical
Part C 11.14

cavity. We then continue with HeNe lasers stabilized


11.14.3 Examples to their gain profile. The next section represents laser ra-
of Frequency-Stabilized Lasers diations that are stabilized to suitable absorption lines
of atoms, molecules, or ions. In view of its practical
This section describes a few examples of stabilized importance, we focus on HeNe lasers, which can be sta-
lasers. The radiations of some of them are recom- bilized to the absorption lines of molecular iodine. The
mended as reference frequencies for the realization of absorbing particles of these lasers are contained in an
the length unit meter and as references for scientific ap- absorption cell. In the next step, laser stabilization sys-
plications [11.2009]. Frequency-stabilized lasers have tems based on atomic or molecular beams are discussed.
been developed covering a wide range of wavelengths The last part of this section presents a brief description
from the near UV to the far IR. Of these examples, HeNe of lasers stabilized to cold ions and atoms.
lasers are of great practical importance since they are of-
ten employed in many applications, e.g., as wavelength Frequency Stabilization of Diode Lasers
standards in interferometers for dimensional metrology. Tunable lasers are important tools in the field of preci-
Most of these lasers utilize the frequency of their gain sion laser spectroscopy. Whereas in the past the visible
profile itself as the reference for the stabilization. In these spectrum was covered mostly by dye lasers, diode lasers
cases, the stabilized frequency depends on the discharge are increasingly taking over due to their small size, high
parameters, the gas pressure, and gas mixture inside the efficiency, high power, and reliability. They are avail-
laser tube and the relative reproducibility is limited to able in a wide range of the visible and infrared spectrum.
some 10−7 . Hence, if the absolute value of the laser fre- However, if high spectral resolution is required, the line
quency is important, it should be compared from time width of most solitary laser diodes, which ranges from
to time with a superior standard, e.g., a HeNe Laser of 10 MHz to 300 MHz, is orders of magnitude too large.
which the frequency is stabilized to an absorption line Several methods have been developed to improve the
of molecular iodine. spectral purity of these lasers. Most of them apply optical
With increasing requirements on reproducibility and feedback [11.2035, 2036]. This section discusses a typ-
accuracy, the laser frequency needs to be stabilized to ical example, where the length of the laser resonator
suitable references such as the narrow absorption lines is increased by an external reflector [11.2037, 2038].
of atoms, molecules, or ions and line broadening caused Compared to solitary laser diodes, the line width of such
by the movement of the absorbers needs to be reduced by extended-cavity diode lasers (ECDL) can be reduced to
Doppler-free techniques such as saturated absorption or some 100 kHz. Figure 11.254 shows two typical setups
of ECDLs in the Littrow and Littman configurations. In
both configurations, the beam leaving the antireflection-
Coarse
a) b) tuning Output coated facet of the laser diode (LD) is collimated and
Output PZT beam directed onto a reflection grating. In the Littrow con-
beam
End mirror figuration (Fig. 11.254a), the laser grating acts as the
Coarse end mirror of the extended laser resonator where the
Collimator tuning Collimator beam is back-reflected into the laser diode in the first
diffraction order. The zeroth-order beam is coupled out.
Coarse frequency tuning can be performed by rotating
LD EOM LD EOM the grating whereas a piezoelectric transducer (PZT)
Grating Grating
and/or an electrooptic modulator (EOM) can be used to
Fig. 11.254a,b Typical setups of extended-cavity diode lasers fine-tune and control the laser frequency by changing
(ECDLs). (a) Littrow configuration, (b) Littman configuration (see the optical length of the cavity. Frequency tuning can
text) also be achieved by changing the injection current of the
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 853

laser diode; this method, however, will also change the for many applications in metrology. Provided the neon
laser power. The Littrow configuration can be designed gas inside the laser tube consists of a single isotope,
to be very compact. Unfortunately, the direction of its the width of the Doppler-broadened gain profile is in
output beam changes with any rotation of the grating. the range of approximately 1.5 GHz and single- or two-
This shortcoming is avoided in the Littman configura- frequency operation can easily be achieved by choosing
tion [11.2039] where the ECDL contains an additional a sufficiently short length of the laser resonator. Ow-
mirror (Fig. 11.254b). In this configuration the beam ing to these favored properties and their simplicity,

Part C 11.14
deflected in the first diffraction order is directed onto frequency-stabilized HeNe lasers were developed very
this extra mirror and back-reflected from there into the early [11.2041]. The first stabilization systems – which
laser diode. In the Littman configuration, the laser beam are still used in many laboratories – apply the gain profile
passes the grating twice and hence the wavelength selec- itself as the frequency reference.
tivity is increased compared to the Littrow configuration.
The output beam leaves the grating in the zeroth order. In Lamb-dip stabilization. The Lamb-dip-stabilized
this configuration, coarse frequency setting is achieved laser was one of the first frequency-stabilized
by rotating the end mirror, with the consequence that lasers [11.2042]. It makes use of the fact that the out-
the direction of the output beam does not change. Fine- put power passes through a local minimum – the Lamb
tuning of the frequency can be performed in the same dip – when the laser frequency is tuned across the center
way as with the Littrow configuration by means of a PZT of the gain curve (Fig. 11.255a). Similar to the Doppler-
or an EOM. free minimum of saturated absorption, the Lamb dip is
The frequency noise of ECDLs occurs at Fourier fre- caused by an increased saturation of the gain at the line
quencies low enough that a further line width reduction center when both the forward- and backward-running
below 100 kHz can be achieved by active frequency sta- waves inside the resonator interact with the same veloc-
bilization to the resonance of an optical cavity [11.2040], ity group (νz = 0) of atoms. Hence the number of atoms
as described in Sect. 11.14.2. Precise frequency tuning contributing to the laser action is decreased, leading to
can be performed, e.g., by changing the length of the a reduced laser power at line center. To generate the error
optical reference cavity. This method, however, strongly signal (Fig. 11.255b), the laser frequency is modulated
perturbs the stability of the cavity. To achieve the high- and the first harmonic in the output power is detected.
est possible resolution, it is better to introduce a variable
frequency difference between the laser output beam and Two-mode stabilization. A simple stabilization sys-
the cavity resonance. Since the frequency-shifted beam tem can easily be set up, if the HeNe laser is operating
is locked to the cavity resonance, which is not affected, at two adjacent longitudinal modes (Fig. 11.256a) and if
the stabilization circuit will shift the laser frequency,
with the consequence that it can be tuned very precisely
Laser power
relative to the stable cavity resonance. Such a shift can
be achieved, e.g., by an acoustooptic modulator or an
electrooptic modulator. Using the PDH technique and
a carefully designed and isolated reference cavity of
ultrahigh finesse, a line width as narrow as 1 Hz was
recently observed, demonstrating the great potential of
diode lasers for applications in precision spectroscopy
and optical frequency standards [11.2021].

Frequency Stabilization of HeNe Lasers Error signal


HeNe lasers can operate at several different wave-
lengths within the spectral range between the green Fig. 11.255a,b
(λ = 543 nm) and the infrared (λ = 3.39 µm). Regard- Tuning curve
ing the various wavelengths, the emission at λ = 633 nm 0 (a) and error
is probably most important. HeNe lasers are advan- signal (b) of
tageous since their operation is simple, the intrinsic a Lamb-dip-
frequency noise is small, and the output power in the Laser frequency stabilized HeNe
range between 100 µW and some 3 mW is sufficient laser
854 Part C Coherent and Incoherent Light Sources

izing beam splitter. Similar to two-mode stabilization,


Laser power Error signal
the difference of the output powers at ν+ and ν− can be
a) b) utilized as the error signal [11.2045].
Alternatively, the error signal can also be generated
A B A by utilizing the frequency difference δν = ν+ − ν− . It
0
has been shown that δν changes with the mean laser fre-
quency and that it has a minimum at the line center. This
Part C 11.14

dependence is caused by nonlinear mode-pulling effects


ín ín+1 in the gain medium. The error signal to find this min-
Laser frequency Laser frequency imum is generated by modulating the laser frequency
and monitoring the beat frequency between the two Zee-
Fig. 11.256a,b Tuning curve (a) and error signal (b) of a two-mode man modes by means of a reversible counter [11.2046].
stabilized HeNe laser To derive the error signal, the direction of counting is
reversed at every half period of the modulation. The ac-
these modes are polarized perpendicular to each other. cumulated counter content, which corresponds to the
These conditions are provided, e.g., in commercial HeNe integrated error signal, is then fed into a digital-to-
laser tubes of 30 cm length with internal mirrors. Per- analog converter after each period. Its output is used
pendicular polarization is observed since it minimizes to control the frequency of the laser so that the mean
the gain competition of two modes. Furthermore, the laser frequency coincides with the minimum of the beat
two planes of polarization are fixed within the tube. frequency. With such lasers a relative frequency repro-
These properties allow us to separate the two modes ducibility of 10−8 can be achieved over a period of five
by a polarization divider, e.g., a Wollaston prism, and months under laboratory conditions [11.2046].
to monitor the power in each mode by a separate pho-
todetector. The difference between the photocurrents of Absolute Frequency Stabilization Utilizing
the two detectors I1 − I2 depends on the frequencies of Separate Absorption Cells
the two modes (Fig. 11.256b). It crosses zero when they As indicated above, the frequency of HeNe lasers stabi-
are distributed symmetrically with respect to the center lized to their gain profile may change with time. Such
of the gain curve and the powers in the two modes are frequency shifts can be reduced by several orders of
identical. Hence, the difference in the photocurrents is magnitude if the frequency reference is provided by
used as the error signal for frequency stabilization and a suitable narrow absorption line of which the transi-
no frequency modulation is necessary [11.2043]. Sev- tion frequency is largely independent on the parameters
eral means can be applied to transfer the control signal of operation. There are now several different laser sys-
to the length of laser tube, such as heating the tube via tems available in a wide range of the optical spectrum
the discharge current or a separate external heater. With which are stabilized to such frequency references. Some
this simple laser stabilization technique, a relative repro- of these have been recommended by the Comité Inter-
ducibility of better than 10−7 has been demonstrated. national des Poids et Mesures (CIPM) [11.2009]. Their
During a time interval of five days relative frequency radiations are listed together with the values of their fre-
variations as low as 10−9 have been demonstrated under quencies, wavelengths, and their relative uncertainties in
favored laboratory conditions [11.2044]. Table 11.56. Six of the recommended reference frequen-
cies are stabilized to hyperfine-structure components of
Zeeman stabilization. Another method of frequency molecular iodine, which has a rich spectrum of narrow
stabilization widely applied in commercial HeNe lasers absorption lines in the visible range. They belong to the
and laser interferometers utilizes the Zeeman effect transition between the electronic B level and the ground
in a short (≈ 10 cm) single-mode laser. If we apply state (X level). Since the iodine molecule is heavy, its ve-
a longitudinal magnetic field, the Zeeman effect causes locity – and hence the Doppler broadening – is rather low
a splitting of the laser mode into two submodes ν+ and at room temperature. Furthermore, the vapor pressure –
ν− of opposite circular polarization and slightly differ- causing a pressure-induced shift and broadening – can
ent frequencies. Depending on the size of the magnetic be controlled conveniently via the temperature of a cool-
field, the frequency difference ν+ − ν− is in the range ing finger attached to the iodine absorption cell. Four of
between 300 kHz and 2 MHz. The two submodes can be the iodine references are used to stabilize HeNe lasers
separated by a quarter-wave plate followed by a polar- at λ ≈ 543 nm, 612 nm, 633 nm, and 640 nm. From this
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 855

Table 11.56 Recommended reference wavelengths/frequencies generated by stabilized lasers [11.2009]


Atom / Transition Wavelength (fm) Frequency Rel. std.
Molecule uncertainty (1 σ)
1 115 In+ 5s2 1 S0 –5s5p 3 P0 236 540 853.54976 1 267 402 452 899.92 kHz 3.6 × 10−13
2 1H 1S–2S (Two-photon transition) 243 134 624.62603 1 233 030 706 593.61 kHz 2.0 × 10−13
3 199 Hg+ 5d10 6s 2 S1/2 (F = 0)–5d9 6s2 2 D5/2 (F = 2) 281 568 867.591969 1 064 721 609 899.143 Hz 1.9 × 10−14

Part C 11.14
∆m F = 0
4 171 Yb+ 6s 2 S1/2 (F = 0)–5d 2 D3/2 (F = 2) 435 517 610.73969 688 358 979 309 312 Hz 2.9 × 10−14
171 Yb+ 4.0 × 10−12
1/2 (F = 0, m F = 0)– F7/2 (F = 3, m F = 0)
5 2S 2 466 878 090.061 642 121 496 772.6 kHz
6 127 I
2 R(56) 32-0, component, a10 532 245 036.104 563 260 223 514 kHz 8.9 × 10−12
7 127 I
2 R(127) 11-5 component a16 (or f) 632 991 212.58 473 612 353 604 kHz 2.1 × 10−11
8 40 Ca 1 S –3 P ; ∆m = 0
0 1 J 657 459 439.29167 455 986 240 494 150 Hz 1.1 × 10−13
9 88 Sr+ 5 2 S1/2 –42 D5/2 674 025 590.8631 444 779 044 095.5 kHz 7.9 × 10−13
10 85 Rb 5S1/2 (Fg = 3)–5D5/2 (F e = 5) two-photon 778 105 421.23 385 285 142 375 kHz 1.3 × 10−11
11 13 C H
2 2 P(16)(ν1 + ν3 ) λ = 1 542 383 712 194 369 569.4 MHz 5.2 × 10−10
3 × 10−12
(2)
12 CH4 P(7) ν3 , component of the F2 3 392 231 397.327 88 376 181 600.18 kHz
central hyperfine structure
13 12 C16 O
2 R(10) (000 1)–(100 0) line of the CO2 -laser 10 318 436 884.460 29 054 057 446 579 Hz 1.4 − 13

group, the one operating at 633 nm is of particular im- 20 cm and 10 cm, respectively, corresponding to a min-
portance since it is used in many standard laboratories imum length of the resonator of approximately 35 cm
as a reference for interferometric length measurements, and a free spectral range of ≈ 430 MHz. Despite of the
laser wavelength calibrations, and applications in pre- rather long resonator the laser emits only one single fre-
cision laser spectroscopy. It can also act as a reference quency, owing to the loss in the absorption cell. In order
to calibrate HeNe lasers that are stabilized to their gain to reduce the influence of acoustics and vibrations, the
profile by beat-frequency comparisons. Hence, the I2 - resonator should be made as rugged as possible. The
stabilized HeNe laser at λ = 633 nm can be regarded as spacers should consist of a material of low thermal ex-
the workhorse in many laboratories. pansion. The radii of curvature of the laser mirrors are
The iodine molecules are contained at low vapor usually in the range r = 0.6–4 m with a radius of r = 1 m
pressure in a cell. Depending on the laser system, the most commonly used. Both mirrors have a reflectivity
length of the cell may range from a few centimeters up of approximately 98%, allowing single-frequency oper-
to several meters. In either case, the content of impuri- ation over most of the free spectral range. Output powers
ties has to be low in order to prevent any frequency shifts of up to 300 µW have been achieved, sufficient for most
caused by collisions with impurities. For example, in the applications in laser spectroscopy and interferometry.
case of iodine-stabilized lasers, the quality of the iodine
filling limits the uncertainty ultimately achievable. Nev-
Photo detector
ertheless, as a result of its rich spectrum, I2 is often used + preamplifier HeNe laser tube
PZT I2 absorption PZT
as the frequency reference for different types of lasers cell
operating within the visible spectrum. Two types of I2 -
Output
stabilized lasers, the HeNe laser (λ = 633 nm) and the
frequency-doubled Nd:YAG laser (λ = 532 nm) will be
discussed in the following. f Modulation
frequency
3f generator
Iodine-stabilized HeNe laser (λ = 633 nm). Fig-
PZT
ure 11.257 schematically shows a typical setup of an driver
iodine-stabilized HeNe laser. The laser head consists
3f PSD Integrator
of a HeNe discharge tube and an iodine absorption filter
cell mounted inside the laser resonator. The lengths of
the discharge tube and the absorption cell are typically Fig. 11.257 Experimental scheme of an iodine-stabilized HeNe laser
856 Part C Coherent and Incoherent Light Sources

The two mirrors are mounted on PZT actuators, allow- The reproducibility of the iodine-stabilized HeNe
ing one to change the resonator length and thereby the laser was investigated by measuring the dependence of
laser frequency by applying a voltage to the PZTs. the laser frequency on the various operation parame-
Figure 11.258a shows four absorption features in the ters and by frequency inter-comparisons between lasers
tuning curve of the laser. They belong to the hyperfine- of different institutes. The laser frequency depends on
structure (HFS) components d, e, f, and g of the transition the modulation width, the iodine vapor pressure, and
R(127), v = 5, v = 11 of 127 I2 . The separation between slightly on the laser power. The coefficients are approx-
Part C 11.14

the components d, e, f, g is approximately 13 MHz and imately −6 kHz/Pa and −10 kHz/MHz for the pressure
the full width at half-maximum of each line is in the and modulation dependence, respectively. International
range of 5 MHz, corresponding to a quality factor of frequency comparisons between iodine-stabilized lasers
Q = ν/δν ≈ 108 . The height is approximately 0.1% of have shown that the stabilized frequencies of the ma-
the laser power. To generate the error signal for the stabi- jority of iodine-stabilized HeNe lasers coincide within
lization, the length and thereby the frequency of the laser a range of approximately 12 kHz, corresponding to
is modulated harmonically by applying a sine-wave volt- 2.5 × 10−11 ν. For specified operation parameters (tem-
age to the left PZT (Fig. 11.257). For the stabilization, perature of the cell: (25±5) ◦ C, temperature of the
third-harmonic detection is used. The third-harmonic cold point: (15 ± 0.2) ◦ C, width of frequency mod-
signal in the output power is filtered out, demodulated ulation between the peaks: (6 ± 0.3) MHz, one-way
by a phase-sensitive detector (PSD) and passed through intracavity beam power: (10±5) mW) a relative stan-
a low-pass filter. It then serves as error signal for the dard uncertainty of the recommended frequency value
stabilization. A typical third-harmonic spectrum of mo- of 2.5 × 10−11 can be achieved [11.2009].
lecular iodine containing seven HFS components within
the tuning range of the laser is shown in Fig. 11.258b. Iodine-stabilized frequency-doubled Nd:YAG lasers
Each absorption feature is suitable as a reference for the (λ = 532 nm). Frequency-doubled YAG lasers pumped
stabilization. by diode lasers are of particular interest in applications
With the servo loop operating, the length of the laser as optical frequency standards for the following rea-
is stabilized such that the third-harmonic signal of the sons. Small lasers providing us with high output powers
corresponding HFS component vanishes at its central of 100 mW at 532 nm are commercially available. The
zero crossing. intrinsic frequency noise of YAG lasers can be very low.
The stability and the reproducibility of the Part of the emission range coincides with strong ab-
I2 -stabilized HeNe laser can be investigated by beat- sorption lines of molecular iodine (Fig. 11.259a) that
frequency measurements of two independent laser are suitable as reference frequencies for the stabiliza-
systems. Figure 11.245 shows the measured Allan stan- tion. Figure 11.259b shows the Doppler-free absorption
dard deviation σ(τ) of an iodine-stabilized HeNe laser spectrum observed within the continuous tuning range
versus the integrating time τ. In the range between of 5 GHz of a commercial laser. The observed absorption
τ = 10 ms and τ = 100 s, σ(τ) decreases approximately lines represent two sets of hyperfine components belong-
with the square root of τ, corresponding to white ing to the 32-0, R(57) and the 32-0, P(54) ro-vibrational
frequency noise. The minimum instability of about lines labeled #1104 and #1105, respectively [11.2047].
2 × 10−13 is observed at an integrating time τ ≈ 1000 s. Any of these transitions is suitable as a frequency
reference. Since the frequency difference to the recom-
mended a10 component of the 32-0, R(56) transition is
a) Outpout power b) Discriminator signal known to about 2 kHz an accurate optical frequency can
j i h gfed be attributed to each HFS component.
22 MHz
Various methods have been used in different lab-
oratories to generate the error signal. The methods of
modulation transfer spectroscopy [11.2048, 2049] and
phase-modulation spectroscopy [11.2050,2051] are very
powerful to achieve discriminant signal with a high
Laser frequency Laser frequency signal-to-noise ratio.
International frequency comparisons show that the
Fig. 11.258a,b Saturation dips (a) and error signals (b) of an iodine- frequency reproducibility of these lasers is in the range
stabilized HeNe laser (λ = 633 nm) of 5 kHz [11.2052,2053], mostly limited by potential im-
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 857

a) T (V) 5 2D3/2, 5/2


5248 nm
1
6 2P1/2, 3/2 778 nm
0.8
D1 D2
5 2P3/2 420 nm
0.6 5 2P1/2
778 nm 795 nm 780 nm

Part C 11.14
0.4
5 2S1/2
0.2
Fig. 11.260 Energy levels of Rb relevant for a two-photon
#1104 #1105
0 stabilized diode laser
–3 –2 –1 0 1 2 3
U (V)
sion band at 1.55 µm. Its optical frequency has been
b) A (V) determined [11.2055].
2.5
In a simple setup [11.2054], the collimated beam of
an extended-cavity diode laser passes through an absorp-
2 R(57) 32-0 P(54) 32-0 tion cell filled with rubidium vapor. The cell is sealed
#1104 #1105 with Brewster windows at its ends and filled with nat-
1.5 ural rubidium (73% 85 Rb and 27% 87 Rb). The beam
is retro-reflected by a mirror or a cat’s eye in order
1 to allow Doppler-free two-photon excitation. Optical
feedback into the diode laser is avoided by Faraday iso-
0.5
lators. When the laser frequency is scanned through the
0
two-photon resonance, the excitation of the upper level
(52 D5/2 ) is observed via the blue fluorescence (420 nm)
–3000 –2000 –1000 0 1000 of the 6P–5S transition in the cascade of the spontaneous
Äí (MHz)
decay 5D → 6P → 5S. With this setup, a frequency sta-
Fig. 11.259a,b Absorption lines of molecular iodine within bility of σ(τ) = 3 × 10−13 τ −1/2 has been achieved for
the emission profile of a commercial frequency-doubled integrating times τ up to 2000 s.
Nd:YAG laser. (a) Doppler-limited, (b) with Doppler-free It is known that the stabilized frequencies of stan-
excitation, the hyperfine structure is resolved dards based on two-photon transitions suffer from light
shifts. Its magnitude depends linearly on the intensity.
purities in the absorption cell. Regarding its high power, Therefore, it is important to control the laser power and
its compactness, and its high frequency reproducibility, to prepare a well-defined laser beam geometry for the
the iodine-stabilized frequency-doubled Nd:YAG laser excitation. This requirement can be fulfilled if the ab-
represents an optical frequency standard with important sorption cell is mounted inside a nondegenerate optical
applications in precision length metrology, interferom- resonator. The use of a resonator also allows a power
etry, and spectroscopy. buildup of the radiation and therefore an increase of
the two-photon excitation. Furthermore, it provides ex-
Laser stabilized to a two-photon transition in act retro-reflection of the laser beam, which is necessary
rubidium. The radiation of a laser stabilized to to suppress residual first-order Doppler shifts. In the
the two-photon transition 5S1/2 –5D5/2 in rubidium experiments [11.2054], the laser frequency was pre-
(Fig. 11.260) [11.2054] represents a reference in the stabilized in a first step to a resonance of this cavity.
near infrared at a wavelength of 778 nm. In this spec- It could then be tuned through the two-photon res-
tral range, easy-to-handle laser diodes of low frequency onance by changing the length of the resonator via
noise are available, allowing the development of a trans- a PZT actuator to which one of the mirrors is mounted.
portable optical frequency standard of high precision. Compared to the results of the simple setup described
Furthermore, the laser may provide a precise fre- before, the observed frequency stability was approxi-
quency reference for optical communication systems mately the same. However the light shift could be better
since twice its wavelength coincides with the transmis- controlled and consequently the frequency of the tran-
858 Part C Coherent and Incoherent Light Sources

sition can be extrapolated more precisely to zero laser of cold atomic hydrogen is formed by guiding hydrogen
power. molecules through a gas discharge and reflecting the
Laser-cooled ensembles of Rb atoms have also been atomic particles at a plate which is cooled by liquid he-
used for frequency stabilization to reduce the influence lium. The reflector directs the hydrogen atoms on the
of the second-order Doppler effect [11.2056]. Further optical axis of an optical resonator which is tuned close
evaluations will show if a standard based on cold Rb to the 1S–2S two-photon transition. The longitudinal
atoms leads to a significant reduction of the relative fre- excitation inside a resonator allows the strong power
Part C 11.14

quency uncertainty. Nevertheless, in its present state, the buildup necessary for a two-photon excitation, precise
Rb-stabilized laser represents an interesting precision mode-matching of the forward- and backward-running
frequency reference. waves inside the resonator, and an increased interaction
time of the atoms with the laser beam, leading to in-
Stabilized Lasers Based creased spectral resolution. The relative uncertainty of
on Atomic or Molecular Beams the transition frequency recommended by the CIPM is
Atomic and molecular absorbers are often prepared in as low as 2.0 × 10−13 [11.2009].
beams rather than in absorption cells for various rea- In the case of single photon transitions, the transvers
sons. First, some gases such as hydrogen are not stable excitation by separated laser fields (Fig. 11.262) is fre-
as atomic species and need to be prepared just shortly quently applied to achieve high spectral resolution
before excitation. Vapors of metals would soon coat the and a good signal-to-noise ratio. It was shown by
cell windows and strongly decrease their transparency. Bordé that this method leads to an atom interferom-
Second, the use of a collimated beam allows us to uti- eter (Ramsey–Bordé interferometer) where the laser
lize an excitation geometry in which the laser beam beams act as coherent beam splitters for the atomic
crosses the atomic beam at a right angle. In the case beam [11.2061–2063]. The prominent advantage of opti-
of single-photon transitions, this may reduce the first- cal Ramsey excitation with separated fields results from
order Doppler effect by several orders of magnitude. the fact that the transit-time broadening and the resolu-
Furthermore, for long-lived atomic states, the excitation tion can be adjusted independently. The former can be
and detection zones can be separated, leading to an in- increased by choosing short interaction times in each
creased signal-to-noise ratio since scattered light from zone, thereby allowing a large fraction of the atoms
the excitation beam can be better suppressed. to contribute to the signal. The resolution, however, is
The mean velocity of molecules or atoms at room mainly determined by the time of flight between the
temperature ranges from approximately 100 m/s to more interaction zones. In the following, we give a brief de-
than 2000 m/s. At this velocity, the interaction time of scription of the Ramsey–Bordé interferometer. Utilizing
the particles crossing the laser beam at a right angle, is the internal energy structure of the atoms, absorption and
typically less than 10−5 s for beam diameters of a few induced emission, processes can be used to split or de-
millimeters. Hence, the corresponding line broadening is flect atomic beams. If an atom absorbs a photon from
more than 0.1 MHz. This broadening can be reduced by a traveling wave, it also absorbs the photon momentum
applying Ramsey’s method of separated field excitation k (Fig. 11.261a). Hence, the excited atom suffers a pho-
first introduced in the microwave range [11.2057]. For ton recoil. If the atomic wave was in the excited state
single-photon transitions in the optical regime, where
the wavelength of the radiation is typically much smaller
than the diameter of the atomic beam, additional steps a) |eñ b) |eñ
need to be taken to use separated field excitation. This
can be achieved either by blocking well-defined tra- |gñ |gñ
jectories of the atomic beam [11.2058] or by using
three [11.2059] or more [11.2060] spatially separated
| e, p + k ñ | e, p + k ñ
excitation zones.
| g, pñ
An alternative method is a longitudinal excitation
where the atoms fly parallel or anti-parallel to the laser | g, pñ | g, pñ
beam. This method is suitable in the case of two-photon | e, p + k ñ
k k
transitions. For example, one of the recommended radia-
tions (Table 11.56) corresponds to the 1S–2S two-photon Fig. 11.261 Laser beams as beam splitters for an atomic
transition of atomic hydrogen. In the experiment, a beam wave
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 859

40
1
P1 Ca

Cooling transition
3
P1
Reference transition

D d D äí = 33 MHz äí = 0.4 KHz

Part C 11.14
ë = 423 nm ë = 657 nm
Fig. 11.262 Ramsey–Bordé matter–wave interferometer 1
S0
(the figure shows only those partial beams that lead to an
interference structure) Fig. 11.263 Partial energy-level diagram of 40 Ca

before interaction with the laser radiation, the inverse the frequencies of the ∆m J = 0 transitions are almost
process (induced emission) will occur (Fig. 11.261b). insensitive to electric and magnetic fields.
The probability ρ of observing such excitation or emis- The inter-combination lines have been investigated
sion process depends on the intensity, the frequency of in effusive beams of magnesium [11.2066], stron-
the light field, and the duration of the interaction. In gen- tium [11.2067, 2068], and barium atoms [11.2069].
eral, the atom will be left in a coherent superposition of Most work for optical frequency standard applica-
the ground and the excited state (Fig. 11.261). Since the tions has probably been performed with Ca atomic
atoms have different momenta in both states, it is more beams [11.2070, 2071]. This transition was investigated
appropriate to use the picture of atomic wave packets. by various groups [11.2064, 2072–2074]. The radiation
The interaction can act, e.g., as a 50% beam splitter of a Ca-stabilized laser is also recommended as a refer-
(ρ = 0.5, π/2 pulse) or as a mirror (ρ = 1, π pulse). In ence frequency by the CIPM [11.2009]. As a typical
any case, the phase of the light beam is transferred to the example let us discuss the layout of a transportable
deflected partial atomic wave. If the light field is slightly Ca-atomic-beam standard (Fig. 11.264) [11.2064].
detuned from the atomic resonance, the corresponding A few milliwatts of the available output power of an
energy difference δω is also transferred to the deflected ECDL – pre-stabilized to a reference frequency of an op-
partial wave as kinetic energy and consequently the tical cavity – is sent through a polarization-preserving
de Broglie wavelength is changed. single-mode fiber to a beam splitter/mirror configura-
The combination of such beam splitters may lead tion and is split into two beams 1 and 2 of equal
to atom interferometers that are similar to an optical power. From each one of the beams (1 or 2) crossing
Mach–Zehnder interferometer (Fig. 11.262). During the
first and each subsequent interaction, the matter wave
is coherently split into partial waves with the internal Photomultiplier
states |g and |e, which are represented by the solid and
the dashed lines in Figs. 11.261 and 11.262. If an ab-
sorption or emission is induced, the momentum of the
corresponding wave packet is changed by the photon
momentum k. At the final interaction, the loop of the D
trajectories closes and the laser field superimposes the d
partial waves, resulting in an atom interference. Since D 1 2
the atomic wave packets leave the two outputs of each in- Laser
ë = 657.46 nm
terferometer in different internal states, the interference Phase Beam
structure can be observed by monitoring the population plate splitter
either in the excited or the ground state.
The inter-combination transitions 1 S0 –3 P1 of the
Ca atomic beam
alkaline-earth atoms are well known to represent ex-
cellent references for optical frequency standards (see, Fig. 11.264 Scheme of a transportable diode-laser fre-
for example, [11.2065] and references therein). They quency stabilized to the 1 S0 –3 P1 inter-combination
exhibit narrow natural line widths of about 0.04 kHz transition by means of separated field excitation of a 40 Ca
(Mg), 0.3 kHz (Ca), and 6 kHz (Sr). In all three cases beam [11.2064]
860 Part C Coherent and Incoherent Light Sources

the atomic beam perpendicularly an excitation geome- or vice versa, Fig. 11.264) and compensated by rotating
try with two pairs of counter-propagating laser beams the phase plate [11.2064].
is obtained by the help of two cat’s-eye retro-reflectors. The phase of each cosine function in (11.240) con-
The co-propagating beams are separated by the distance tains three contributions. Besides ΦL there are the terms
D = 10 mm and the distance between the two innermost ∆0 resulting from the detuning, δrec = k2 /(2m Ca c2 )
counter-propagating beams is d = 13 mm. The optical from the photon recoil where k is the wavevector of
layout with the fused silica block is designed in such the laser field and m Ca the mass of a Ca atom, and
Part C 11.14

a way that the part 2 leads to the same excitation geom- ω0 ν2 /(2c2 ) from the second-order Doppler effect.
etry as part 1, but its direction with respect to the atomic The signal for each velocity group ν consists of two
beam is reversed (Fig. 11.264). During the experiment, cosine functions with a period 1/(2T ) that is determined
the laser beams are propagating either in direction 1 or 2 by the distance D and the atomic velocity. The two
and the beams propagating in the opposite direction are components are separated by the recoil splitting 2δrec =
blocked. 2π23.1 kHz. For an optimum superposition of the two
The excited atoms are detected by measuring the flu- cosines, the period should be an integer fraction of the
orescence intensity from the decay of the excited atoms recoil splitting. The FWHM line width of the signal is
by a photomultiplier. The detected fluorescence intensity approximately given by 1/(4T ).
of the ∆m j = 0 transition versus laser frequency detun- From the measured fluorescence signal versus de-
ing ∆ω/2π = (ω − ωg )/2π, representing the frequency tuning δν = ν − νo (Fig. 11.265) one clearly recognizes
difference between the laser frequency ω/2π and the in the central part of the saturation dip the two cen-
frequency ω0 /2π of the Ca inter-combination line, can tral minima of the two cosine terms separated by the
be described by the expression [11.2060]. recoil splitting. With increasing detuning the cosine
structure is washed out, since all velocity groups ν of
I(∆0 ) the atomic beam contribute with a slightly different pe-
∞ riod. The inset of Fig. 11.265 shows the total detected
= A(P, ν, ∆0 ) f (ν) signal where the Doppler broadening is determined by
0
the degree of collimation and the velocity distribution
   of the atomic beam, leading to a FWHM of the struc-
ω0 ν2
× cos 2T ∆0 + δrec + + ΦL ture of 7.5 MHz. With an evaluated relative uncertainty
2c2 of 1.3 × 10−12 combined with a relative stability of
   
ω0 ν2 σ(τ) = 9 × 10−13 at τ = 1 s, the transportable Ca fre-
+ cos 2T ∆0 − δrec + + ΦL dν quency standard is one order of magnitude superior to
2c2
+ B(P, ∆0 ) . (11.240)
Fluorescence signal
In (11.240), A(P, ν, ∆0 ) describes the contribution of
a particular atom with velocity ν to the signal, and 7.5 MHz
B(P, ν, ∆0 ) describes the amplitude of the background
of the Doppler-broadened line including the saturation
dip, both depending on the laser power P and weakly on
the detuning δν = ∆0 /2π of the laser frequency. The fac-
tor f (ν) represents the velocity distribution, where we
have neglected the influence of the velocity components
perpendicular to the atomic beam.

ΦL = Φ2 − Φ1 + Φ4 − Φ3 (11.241)

is a residual phase between the four exciting laser beams 23.1 kHz
having the phases Φi in the interaction zone, and T =
D/ν is the flight time of the atoms between two co- –80 –40 0 40 80
í – í0 (kHz)
propagating beams. The phase ΦL – which shifts the
frequency of the interference structure – can be detected Fig. 11.265 Atom interference structures observed in a ther-
by reversing the directions of the laser beams (from 1 to 2 mal beam of Ca atoms [11.2064]
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 861

the widely used transportable iodine-stabilized HeNe 1


D[5/2]5/2
laser at λ = 633 nm. 3
D[3/2]1/2

Optical Frequency Standards Based


2
on Laser-Cooled Absorbers P1/2 638 nm
935 nm
In the case of frequency-stabilized lasers utilizing
thermal absorbers, the uncertainty in the center of 2
D5/2

Part C 11.14
the reference line is ultimately limited by frequency
shifts caused by residual phase errors in the opti- 369 nm 2
D3/2
cal excitation and by the second-order Doppler shift
δν/ν = −ν2 /(2c2 ). Both frequency shifts scale with the 411 nm
2
F7/2
velocity of the absorbers and can be reduced by orders
of magnitude if the control signal is only generated by 435 nm 467 nm
slow absorbers. In addition, the increased interaction
time of the atoms with the laser beam leads to reduced 2
S1/2
broadening of the reference line. Hence, the most ac-
curate optical frequency standards are based on cold Fig. 11.267 Simplified energy-level diagram of 171 Yb
absorbers. Two typical examples are described in the
following subsections. The first describes a standard uti- below resonance and the cooling occurs by repeated ab-
lizing a single trapped Yb+ ion whereas the second part sorption and emission [11.2077, 2078]. When the clock
presents a frequency standard based on an ensemble of transition is probed, the cooling radiation has to be
cold Ca atoms. turned off in order to suppress light shifts and strong
line broadening. The RF trapping field, however, may
Optical frequency standards based on cold, stored stay unchanged, allowing ideally unlimited interroga-
ions. The ideal reference for an optical frequency stan- tion times. If several ions are confined in a trap, their
dard would consist of an ensemble of identical but repelling forces will lead to an ion cloud, extending into
independent atoms at rest in free space. This condition the nonvanishing RF field and kinetic energy from the
can be approximated in part by a single ion confined oscillating trapping field will be picked up. Such heat-
in a small volume inside an axially symmetric configu- ing can be avoided if only a single ion is trapped in
ration of electrodes shown schematically in Fig. 11.266 the center of the trap, where the trapping field vanishes.
(Paul trap) [11.2075]. Trapping is performed by apply- Since only one ion can contribute to the stabilization, it
ing a suitable RF voltage to the electrodes. Such traps is important to detect the excitation of the reference tran-
allow us to store and cool single ions in the field-free sition with high efficiency. An efficiency close to 100%
region of the trap center.
Ions suitable for precision frequency standards pro-
Excitation probability
vide a closed transition for cooling and a reference 0.8
(clock) transition. Cooling of the ion is performed by
irradiating it with laser radiation which is tuned slightly

30 Hz
Endcap 0.4

Ring
electrode r0 Ö
z0

0
Endcap –120 –60 0 60 120
Detuning

Fig. 11.266 Electrode configuration of an RF ion trap (Paul Fig. 11.268 Absorption signal of a single trapped and
trap) [11.2075] cooled 171 Yb+ ion [11.2076]
862 Part C Coherent and Incoherent Light Sources

of optical frequency standards based on cold stored


Cooling/trapping Reference transition Detection
ions.

15 ms T T Frequency standards based on cold neutral atoms.


Neutral atoms can be cooled and trapped in a magne-
t tooptical trap (MOT) [11.2087] if they have a suitable
cooling transition. In contrast to ions, a large number of
Part C 11.14

atoms in the range of 107 can be utilized to contribute to


Fig. 11.269 Time sequence of atom cooling and trapping the stabilization, leading to an increased signal-to-noise
and probing of the reference transition ratio. However, to avoid unwanted frequency shifts, all
trapping fields have to switched off when the reference
can be accomplished by the method of electron shelv- transition is probed. Hence, the interaction time of the
ing [11.2079], which utilizes the fact that the strong free atoms released from the trap is limited by their
fluorescence on the cooling transition is interrupted if acceleration in the gravitational field.
the ion is excited to the upper state of the reference Candidates for cold-atom optical frequency stan-
transition. dards are silver [11.2088] and the alkali-earth atoms
Several different ions are being investigated for ap- magnesium [11.2089, 2090], strontium [11.2091, 2092],
plications in frequency-stabilized lasers. Very promising and calcium [11.2065, 2070, 2088]. As a typical exam-
results have been observed with standards based on the ple, we describe a frequency-stabilized laser based on
ions of mercury [11.2080], strontium [11.2081, 2082], cold neutral calcium atoms.
indium [11.2083], and ytterbium [11.2076, 2084]. As Besides of the narrow reference transition 1 S0 –3 P1
a typical example, we consider an optical standard at λ = 657 nm (Fig. 11.263), 40 Ca has a strong cool-
based on a single 171 Yb ion (Fig. 11.267). There are ing transition 1 S0 –1 P1 (λ = 423 nm) that can be used to
three different clock transitions that can be accessed cool and trap Ca atoms in a MOT [11.2093]. On this
by the frequency-doubled radiation of diode lasers. The transition, the Ca atoms can be cooled to approximately
435 nm clock transition has recently been observed 3 mK. Further cooling to several mikrokelvin can then be
with a line width as narrow as 30 Hz (Fig. 11.268). achieved in a second step by means of the narrow inter-
In the meantime, this linewidth could be further re- combination transition 1 S0 –3 P1 utilizing the method of
duced to 10 Hz [11.2085]. Utilizing this reference line quench cooling [11.2094].
a relative uncertainty of 9 × 10−15 has recently been In order to achieve high spectral resolution combined
estimated [11.2086], demonstrating the great potential with a good signal-to-noise ratio (SNR), the method of
separated field excitation in the time domain can be ap-
plied, similar to the spatially separated field excitation of
Fluorescence 657 nm
Signal an atomic beam. Short pulses of 1 µs duration are used
1 to excite a significant part of the cold ensemble of atoms.
47 The necessary high spectral resolution is then achieved
by a sufficiently large time separation T between two
consecutive pulses. If the lengths of the pulses are small
compared to their separation, the width of the inter-
–6 –4 –2 0 2 4 ference fringes δν = 1/(4T ) is inversely proportional
í – íCa (kHz) to T .
Cooling and trapping of the atoms and prob-
ing of the clock transition are performed sequentially
(Fig. 11.269). After the atoms have been trapped and
cooled for about 15 ms in the first step, the trapping
fields (laser beams and magnetic quadrupole field) are
switched off, a small homogeneous magnetic quantiza-
–2 –1 0 1 2 tion field (Helmholtz field) is turned on and the clock
Äí (MHz)
transition is probed by two pulsed pairs of counter-
Fig. 11.270 Interference structure of cold, free Ca atoms generated propagating laser beams (Fig. 11.269). During this time,
by time-separated excitation the cloud of cold, free Ca atoms expands according to
Lasers and Coherent Light Sources 11.14 Frequency Stabilization of Lasers 863

the temperature of about 3 mK at a root-mean-square ve-


locity of vrms ≈ 80 cm/s. In the third step, the excitation a) ÄÖgpo
to the 3 P1 state is detected by observing the fluorescence
of its spontaneous decay to the 1 S0 ground state.
If the laser frequency is tuned across the atomic
Time
resonance, the fluorescence intensity contains a contri-
bution that oscillates with the cosine of the laser detuning Ät = 1/f rep

Part C 11.14
(Fig. 11.270). Similar to spatially separated field ex-
citation, this oscillating behavior can be explained by b)
í (m)
an atom interference generated by the excitation with
time-separated fields [11.2093].
f rep
The error signal for the stabilization is generated
from the interference signal by modulating the laser í(0) Frequency
frequency and simultaneously measuring the fluores- í=0
cence intensity. In the most straightforward approach,
the frequency is square-wave modulated between two Fig. 11.271a,b Signal of a mode-locked fs laser, shown
discrete values with the mean frequency tuned close to (a) in the time domain and (b) in the frequency domain
the center of the central fringe. The difference in the
corresponding fluorescence intensities is used as the er-
ror signal. This method corresponds to a first-harmonic laser [11.2098–2101]. Such lasers emit a continuous
detection (1f method) of a servo-control system using train of very short pulses covering a wide range of the
analog electronics and harmonic modulation. The max- optical spectrum of some 100 THz. This range can be
imum slope is obtained for a total modulation width further increased to more than one octave utilizing the
of δνmod = 1/4T , i. e., if the frequency alternates be- phase modulation induced by the pulsed laser beam in
tween the points of maximum slope of the interference an optical fiber of low dispersion [11.2102].
signal. After detection, the error signal is used to step In the frequency domain, the continuous train of fem-
the frequency of the laser spectrometer which corre- tosecond pulses (Fig. 11.271a) corresponds to a comb
sponds to a digital integrating servo control. The linear of frequencies of which the inverse of the pulse sep-
drift of the eigenfrequency of the reference resonator aration is equal to the pulse repetition frequency f rep
can be determined by the servo control and compen- (Fig. 11.271b). The value of an arbitrary comb frequency
sated for by adding a corresponding feedforward signal ν(m) is determined by
to the signal controlling the laser frequency. Using Ca
ν(m) = ν(0) + m f rep , (11.242)
atoms, cooled on the 1 S0 –1 P1 transition to approxi-
mately 3 mK, a relative uncertainty of δν/ν ∼ = 2 × 10−14 where m is an integer representing the respective or-
has been determined [11.2095]. der number of the comb frequency ν(m) and f rep is
the repetition frequency (Fig. 11.271b). Since the group
11.14.4 Measurement velocity and the phase velocity of the short light pulses
of Optical Frequencies circulating in the laser cavity are slightly different an ex-
trapolation to m = 0 leads to the frequency ν(0) which
In many cases, the use of frequency-stabilized lasers – in general – does not coincide with the zero frequency
requires precise knowledge of their frequencies. They (Fig. 11.271b). According to (11.242), the determination
have to be determined in relation to the primary stan- of an arbitrary frequency ν(m) requires the knowledge
dard of time and frequency, the Cs atomic clock. Earlier of f rep , the integer m, and ν(0). The pulse repetition fre-
concepts of optical frequency measurements used a har- quency f rep can be measured phase-coherently against
monic frequency chain of several lasers [11.2096]. For the primary standard of time and frequency. If f rep is
example, measurements of the Ca inter-combination larger than approximately 100 MHz it can easily be iden-
line with such harmonic chain led to a fractional un- tified by an interferometric wavelength measurement of
certainty of 2.5 × 10−13 [11.2097]. In the meantime moderate relative uncertainty (≤ 10−7 ). In order to mea-
alternative powerful methods have been developed to sure ν(0), we take advantage of the fact that the comb
determine optical frequencies. An elegant and success- spans over a frequency range of more than one octave.
ful method is based on a mode-locked femtosecond This allows us to frequency double the low frequency
864 Part C Coherent and Incoherent Light Sources

part of the comb spectrum 2ν(0) + 2m f rep and beat uncertainty of the comb generator itself can still be
it against the corresponding high-frequency part of the neglected.
comb spectrum ν(0) + n f rep . This self-referencing of the
frequency comb leads to a beat 11.14.5 Conclusion and Outlook
 
δν = 2ν(0) + 2n f rep − ν(0) + mνrep The aim of this chapter was to review the foundations
= ν(0) + (2n − m) f rep (11.243) and methods of laser frequency stabilization including
Part C 11

modern methods of optical frequency measurements.


that contains ν(0) plus integer multiples of the pulse Regarding the wide field of lasers, laser spectroscopy
repetition frequency f rep . Since m, n and f rep are and frequency stabilization and the fast development in
known, ν(0) can now be measured with very low un- these fields, this chapter could not be comprehensive
certainty [11.2099, 2100]. Hence, any comb frequency within the limited space available. However, we hope
ν(m) can now be connected phase-coherently to the that it presents a reasonable overview and gives some
frequency of the primary standard of time and fre- introduction to those scientists who are entering the fas-
quency, the Cs atomic clock. Therefore, we can conclude cinating field of laser frequency stabilization and laser
that the frequency of any other laser emitting within spectroscopy.
the spectral range of the frequency comb can also be The examples of stabilized lasers in Sect. 11.14.3
determined phase-coherently by measuring the beat be- are discussed to illustrate the variety of methods ap-
tween the laser frequency and a corresponding comb plied in this field. The development of stabilized lasers
frequency ν(m). Femtosecond lasers have been applied is still progressing in various directions. One is the de-
for the first time to measure the frequency measurements velopment of efficient, reliable and small lasers, e.g.,
of 1S–2S two-photon transition in hydrogen, leading diode lasers, diode-pumped solid-state lasers, or optical
to the recommended value of the frequency given in parametric oscillators (OPOs), which may be impor-
Table 11.56 [11.2098]. tant to achieve efficient, reliable long-term operation.
In the meantime femtosecond lasers are widely Another branch is the design of stable optical refer-
used for optical frequency measurements in many ence resonators to further decrease the laser line width
laboratories worldwide. The first experiments applied close to the quantum limit. An important task is to iso-
titanium-sapphire femtosecond lasers as frequency late them from seismic influences and environmental
comb generators. They are now going to be replaced disturbances. Here, alternative novel methods are be-
by femtosecond fibre lasers in view of their high re- ing developed to compensate and reduce the seismic
liability,ease of operation, and accuracy [11.2103]. It influence. A further reduction of the frequency uncer-
has been shown that frequency comb generators based tainty can be envisaged from the refinement of laser
upon fs lasers are well suited for optical frequency cooling. The introduction of optical frequency combs
measurements of the lowest possible uncertainty. Fur- created by mode-locked fs lasers has provided us with
thermore, it was demonstrated that frequency ratios a universal tool to determine optical frequencies and op-
could be determined with fs lasers with relative uncer- tical frequency ratios. This field will certainly be further
tainties as low as 10−18 [11.2104]. Basically, in their explored by the development of frequency combs oper-
present state, frequency comb generators based on fs ating continuously over long periods and by increasing
lasers allow the measurement of optical frequencies the total width of their emission ranges. It is expected
with uncertainties determined only by the uncertainty that the combination of all these efforts will lead to op-
of the primary standard of time and frequency and tical frequency standards and clocks of unprecedented
the reproducibility of the stabilized laser whereas the low uncertainty.

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Part C 11
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Part C 11
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