Femtosecond lasers

Istvn Robel

Department of Physics and Radiation Laboratory
University of Notre Dame

June 22, 2005

Basics of lasers
Generation and properties of ultrashort pulses
Nonlinear effects:
second harmonic generation
white light generation
Amplification of short laser pulses
Ultrafast laser spectroscopy

Outline
Absorption Spontaneous emission
Ground state
Ground state
Characteristics of spontaneous emission
Random process
Photons from different atoms are not coherent
Random direction of emitted photon
Random polarization of emitted photon
Spontaneous emission
Two types of particles in nature: bosons and fermions
Bosons
Examples: photons, He
4

atoms, Cooper pairs
A quantum state can be
occupied by infinite many
bosons
Bose-Einstein condensation:
all bosons in a system will
occupy the same quantum
state (examples:
supeconductivity, superfluid
He, laser)
integer spin
Fermions
Examples are: electrons,
protons, neutrons, neutrinos,
quarks
Pauli exclusion principle:
every quantum state can be
occupied by 1 fermion at
most
Half-integer spin
Bosons and fermions
Ground state
The emitted photon is in the same quantum state as
the incident photon:
same energy (or wavelength),
same phase (coherent)
same polarization
same direction of propagation
Stimulated emission
E
n
e
r
g
y

Population Inversion
Molecules
Negative
temperature
Light amplification by stimulated
emission occurs when passing
through gain medium

I
0
I >I
0
Competing processes:

Absorption: only possible if an
atom is not in the excited state
Spontaneous emission: important
if the lifetime of the excited state is
too short
Amplification of light
The four-level
system is the
ideal laser
system.
fast
fast
slow
Molecules
accumulate in
this level,
leading to an
inversion with
respect to
this level.
Laser
transition
Four-level laser
Mirror,
R = 100%
Mirror,
R < 100%
I
0
I
1
I
2
I
3
Laser medium in
excited state
I
output
General characteristics of laser radiation:
Coherent (typical coherence length 1m)
Monochromatic (A/=10
-6
)
Directional (mrad beam divergence )
Polarized
Basic components of a laser
Shortest event ever measured (indirectly): decay of tau-lepton
0.4x10
-24
s
Period of nuclear vibrations: 0.1x10
-21
s
Shortest event ever created: 250 attosecond (10
-18
s) x-ray
pulse (2004)
Bohr orbit period in hydrogen atom: 150 attoseconds
Single oscillation of 600nm light: 2 fs (10
-15
s)
Vibrational modes of a molecule: ps timescale
Electron transfer in photosynthesis: ps timescale
Period of phonon vibrations in a solid: ps timescale
Mean time between atomic collisions in ambient air: 0.1 ns
(10
-9
s)
Period of mid-range sound vibrations: ms

Time scales in nature
Long pulse
Short pulse
Irradiance vs.
time
Spectrum
time
time
frequency
frequency
Heisenberg uncertainty principle:

At-Av1
e.g. for a 150fs pulse:
Av=7THz (e.g. v=600THz @ =500nm)
A=6nm wavelength spread @ =500nm

Ultrashort laser pulses
L
c
2
= Au
Frequency modes of the laser cavity
due to the spatial confinement:



e.g. for a 1m long cavity:
Av=1.5GHz
AE=0.6eV
A=0.001A
Frequency modes of the laser cavity
Generation of short pulses by mode-locking
The polarization of very high intensity pulses is rotated when
passing through a nonlinear medium

Using a polarizer low energy pulses can be filtered out, only the
high energy mode-locked pulse gets amplified
Nelson et al Appl. Phys. B 65, 277-294 (1997)
Mode-locking by non-linear polarization rotation
In a medium different frequencies propagate with different velocities
v v / 1
g phase
dn
n d
e
e
| |
= +
|
\ .
Group velocity dispersion: Chirp
Spatial separation of different frequencies
Longer optical path for the frequencies that are ahead
Recombination of different frequencies in a short pulse
Pulse compression
Laser
oscillator
Amplifier
medium
pump
Energy
levels
Difficulties:
beam only passes once through amplifier medium
Output intensity is changing in every roundtrip and
intensity is lower than in cavity

R=100% R<100%
Output
Amplification of short laser pulses
The Pockels cell is a material that rotates the polarization of light if
a voltage is applied on it
If V = 0, the pulse
polarization doesnt
change.
If V = V
p
, the pulse
polarization switches to its
orthogonal state.
V
Pockels cell
Polarizer
R=100% R=100%
Pockels cell and cavity dumping
M mirror
TFP thin film polarizer
FR Faraday rotator
PC Pockels cell

Amplification of the seed pulse:

Seed pulse has to be injected
when gain is maximal
Has to be ejected when pulse
height and stability is maximal
Regenerative amplifier
Oscillator
Stretcher Amplifier Compressor
Pulse is stretched first to avoid high intensity artifacts in the amplifier

Amplified pulse is compressed to obtain the short pulse duration
Chirped Pulse Amplification
Higher frequencies occur due to the
non-linear response of the material at
high intensities
(2 ) ( ) n n e e =
Phase matching condition
ensures conservation of
momentum:


Nonlinear polarization:
P=c(_
1
E+_
2
E
2
+...)





t E t E P e c_ e c_
2
0 2 0 1
cos cos + =
t t e e 2 cos
2
1
2
1
cos
2
+ =
t E E e cos
0
= For a photon:
Second harmonic!
Nonlinear Optics
0 2
( , ) ( ) z t k z n I t | ~
0 2
( , ) ( )
( )
inst
z t I t
t k z n
t t
|
e
c c
= =
c c
775 nm, 150 fs pulse in
sapphire crystal
A wide range of frequencies is
generated with a short, intense
pulse
Self phase modulation and white light continuum
Wavelength, nm
I
n
t
e
n
s
i
t
y
,

a
u

Parameters:
Wavelength of fundamental: 775 nm
Pulse duration: 150 fs
Pulse energy: 1mJ
Power per pulse: 7 GW
Repetition rate: 1KHz
Wavelength of second harmonic: 387 nm
Pulse duration: 150 fs
Pulse energy: 0.25mJ
Er doped
fiber oscillator
25KHz
=1.55m
Pumped with
Cw diode laser
=1m
P=150mW
Pulse
compressor
Second
Harmonic
Generation
Pulse
Stretcher
First Level
Nd:YAG pump laser
Ti:Sapphire
Regenerative
amplifier
Pockels cell
with
HV supply
and delay timer
Pulse
compressor
Second and
Third
harmonic
Second Level
Output
The Clark CPA-2010 Laser System
Unexcited medium Excited medium
Unexcited
medium
absorbs
heavily at
wavelengths
corresponding
to transitions
from ground
state.
Excited
medium
absorbs
weakly at
wavelengths
corresponding
to transitions
from ground
state.
Varying the delay between excitation pulse
and probe pulse results time-dependent
measurement of phenomenon
Time resolution is limited by the length of
the excitation pulse
Transient absorption spectroscopy

To PC
Optical Delay Rail
Frequency
Doubler
Ocean Optics
S2000 CCD Detector
Sample
Cell
Filter Wheel
Chopper
CLARK
-MXR
CPA-2010
775 nm, 1 kHz
1 mJ/pulse
(7fs -1.6 ns)
Probe
Pump
Ultrafast Systems
Sample is excited by short laser pulse (pump)
Differential absorbance of the sample is measured by a delayed second
pulse (probe)
Time dependence is measured by changing the delay of the probe pulse
Experimental Setup: Pump-Probe configuration
Femtosecond Transient Absorption Spectroscopy at NDRL
Time dependent measurements of:

Thermalization of hot electron in a metal or
semiconductor
Electron-phonon heat transfer
Decay of surface plasmon oscillations
Quantum beats
Electron transfer processes
Exciton lifetime in semiconductors
Charge carrier relaxation in semiconductors
Electron- and energy transfer in molecules
Photoinduced mutations in DNA

Applications of pulsed lasers
R. Trebino, Frequency-resolved Optical Gating: The Measurement of Ultrashort Laser Pulses,
Book News Inc., (2002)

R. Trebino, Lectures in Optics (Georgia Tech Lecture Notes)

K. Ekvall, Time Resolved Laser Spectroscopy, Ph.D. Thesis, RIT Stockholm, (2000)

B. B. Laud, Lasers and Non-Linear Optics, Wiley, (1991)

CPA 2010 Users Manual, Clark-MXR Inc, (2001)

W. Demtrder, Laser spectroscopy, Springer, 1998

Ultrashort Laser Pulse Phenomena
Resources and References