Appl. Phys.
B 65, 313–328 (1997)
Invited paper
Spatial coherence of short wavelength high-order harmonics
T. Ditmire1 , J.W.G. Tisch1 , E.T. Gumbrell1 , R.A. Smith1 , D.D. Meyerhofer2 , M.H.R. Hutchinson1
1 Blackett Laboratory, Imperial College of Science Technology and Medicine, London SW7 2BZ, United Kingdom
2 Department of Mechanical Engineering, University of Rochester, Rochester, New York 14627, USA
Received: 12 May 1997
Abstract. Nonperturbative high-order harmonic conversion
of high-intensity, ultrafast laser pulses in gases represents
a unique means to generate high-brightness, coherent XUV,
and soft X-ray radiation. We review the physics controlling
the spatial qualities of harmonic radiation and recent experi-
mental measurements of high-order harmonic spatial profiles.
We also examine the factors controlling the spatial coherence
of the harmonics. A detailed series of Young’s two-slit experi-
ments that measure the spatial coherence of the harmonics is
presented. These measurements indicate that the harmonics
exhibit good fringe visibility and high spatial coherence.
PACS: 42.65.Ky; 42.25.Kb
Since the first observation of nonperturbative high-order har-
monic generation of laser light in a gas by McPherson et al.
in 1985 [1], high-order harmonics have received considerable
attention as a potential high brightness, coherent source of
X-rays [2]. High-order harmonics are produced when a high
intensity laser is focused into a gas, and the nonlinear os-
cillations of the atoms in the medium re-emit photons at
odd harmonics of the incident laser light. Though low-order
harmonics, such as those with harmonic order less then the
seventh or ninth, have been studied for many years [3], the
experiment of [1] and many others that followed soon after
illustrated that at high intensities (> 1013 W/cm2 ) the expo-
nential drop in yield with increasing harmonic order usually
associated with a lowest-order perturbation theory treatment
does not continue with higher harmonic orders [4–7]. Instead,
above a low order the harmonic spectrum exhibits a plateau of
many harmonics with roughly equal yield, which can reach to
very high orders. For example, harmonics as high as the 155th
order have been observed from the harmonic conversion of
800 nm light in helium [8]. These very high-order harmon-
ics have wavelengths that stretch into the XUV and soft X-ray
region.
The high-order harmonics may represent a very attractive
source of short wavelength radiation. The extensive research
of high-order harmonic generation has been motivated by
C Springer-Verlag 1997
the potential of using these harmonics as a source of high-
brightness, coherent, soft X-ray radiation. A number of recent
experiments have explored the possibility of using the har-
monics in various applications requiring short pulses of XUV
or soft X-ray radiation. Haight et al. have used harmonics
in time resolved pump probe photoelectron spectroscopy of
GaAs [9, 10]. Balcou et al. utilized harmonics in photoioniza-
tion spectroscopy of noble gases with photon energy as high
as 100 eV [11] and Larsson et al. exploited the short pulse na-
ture of the harmonics to measure the lifetime of the 1s2 p 1P
state in helium [12]. XUV harmonics have also been used to
probe the dynamics of laser plasmas [13].
Aside from these applications, the properties of these har-
monics have been very carefully studied by a number of
groups around the world in recent years [4, 5, 14, 15]. Probing
the shortest wavelengths attainable with harmonic generation
has been a topic of extensive research. In addition to the
155th harmonic of a Ti:sapphire laser, the 141st harmonic
from a 1 ps, 1054 nm laser has been observed [16] and the
37th harmonic of a 248 nm KrF laser has been reported [17].
The harmonic spectra that result in most experiments typi-
cally have a number of important features in common. The
harmonic yield drops exponentially over the first few orders
(up to the 7th or 9th). This drop is followed by a long plateau
of roughly constant yield between harmonics, which is in turn
followed by an abrupt cutoff. Theoretical and experimental
studies of this behavior indicate that the location of the har-
monic cutoff, and hence the shortest wavelengths achievable,
is usually given by a universal scaling law [18–20]:
hωcut ≈ Ip + 3.2Up , (1)
where Ip is the atom’s ionization potential, Up is the pon-
deromotive field of the laser, and hωcut is the cutoff harmonic
photon energy. This law has been confirmed in many experi-
ments though some deviations from this scaling have been
observed [21, 22].
Other properties of the high-order harmonics have been
studied as well. The energy yields and conversion efficiency
of the harmonics have been measured. Yields as high as 60 nJ
in the 200 Å wavelength range have been reported [23]. The
314
spectral bandwidth properties have also been examined, in-
dicating that the harmonics exhibit linewidths comparable
to or larger than perturbation theory estimates for the trans-
form limited bandwidth [21, 24]. Recently techniques have
also been developed to measure the harmonic pulse width
as well [25–28]. These studies have confirmed that the har-
monic pulse width is close to that of the driving laser and
therefore using femtosecond laser pulses, soft X-ray pulses
of under 100 fs can be generated. Glover et al. measured the
harmonic pulse width by cross correlating the harmonic with
the laser pulse by using photoionization [26]. This measure-
ment indicated that the spatially integrated harmonic pulse
width from a 100 fs laser varied from 80 to 300 fs, depending
upon the conditions. Similar results have been obtained using
ionization gated absorption [27]. Tisch et al. have also meas-
ured the harmonic pulsewidths from 1 ps laser pulses by using
chirped pulse temporal spectroscopy and have found that if
the pulses are not spatially integrated, the harmonic pulse can
be substantially shorter then the drive laser pulse [28]. In add-
ition to these studies of harmonics produced in gases of single
atoms, the properties of harmonics produced in molecules
[29, 30] and clusters [31] have also been examined in experi-
ments. Recently harmonics produced from laser interactions
with solid target plasmas are beginning to receive attention as
well [32].
Aside from these experiments, there is particular interest
in the spatial properties of the high-order harmonics. Knowl-
edge of the spatial divergence of the harmonics is important
if the harmonics are to be used in applications. It also serves
further to illuminate the nature of the physics controlling the
harmonic generation. In addition, characterization of the spa-
tial coherence is of particular importance if harmonics are
to be used in interferometric applications. The coherence of
high-order harmonics is expected to be high since the ra-
diation is created by the parametric conversion of coherent,
single spatial mode, laser radiation. Measurements of the har-
monics’ far-field profiles have indicated that the harmonics
largely preserve the low divergence, Gaussian character of the
laser radiation [33–35]. However, a more fundamental ques-
tion is whether the high-order harmonics preserve the high
spatial coherence of the fundamental laser radiation.
Until recently, the spatial coherence of the harmonics had
not been measured [36]. While a number of previous experi-
mental studies have characterized the far-field profiles of the
high-order harmonics, knowledge of the far-field profile alone
does not indicate the actual transverse spatial coherence of
the radiation. Measuring the transverse coherence requires
performing some manner of interference experiment such as
a Young’s two-slit experiment. Previously, such techniques
have been applied to measure the spatial coherence of short
wavelength XUV [37] and soft X-ray lasers [38–40] as well
as laser-plasma X-ray sources [41] and low-order harmonics
from solid target plasmas [42].
In this article, we briefly review the equations governing
the propagation of the harmonic field in a nonlinear medium,
and discuss the physics important in determining the har-
monics’ far-field profiles. This is followed by a brief review
of the experiments that have examined the harmonics’ spa-
tial profiles. We then discuss the physics of spatial coherence
in the context of harmonic generation. Finally, we present
a detailed experimental study of the harmonics’ spatial co-
herence. In particular, we have conducted a series of Young’s
two-slit experiments to measure the spatial coherence of soft
X-ray, high-order harmonics in the 270 Å to 480 Å wave-
length range. In general, we find that these harmonics exhibit
good fringe visibility and high spatial coherence.
1 Harmonic production in a nonlinear, ionizing medium
To investigate the physical mechanisms affecting the spatial
properties of the high-order harmonic production, it is useful
to examine the propagation equations governing the build-up
of the harmonic field in a nonlinear medium driven by the
intense laser pulse. Because the efficiency of the harmonic
process is generally low, we can usually ignore any pump de-
pletion on the fundamental laser beam. We also consider laser
pulses that have pulses widths much greater then the time
scale of a single wavelength. This fact allows us to use the
slowly varying envelope approximation in deriving the wave
equation governing the harmonic’s growth [2].
In the slowly varying envelope approximation, the wave
equation for the qth harmonic’s field oscillating at a frequen-
cy ωq is
n 2q ω2q 4πω2q
∇ 2 Aq + Aq = − Pq , (2)
c2 c2
where Aq is the field strength of the qth harmonic, n q is the
spatially and temporally varying refractive index of the me-
dia at ωq , and Pq is the polarization induced by the laser field
at a frequency ωq . Equation (2) ignores the group velocity
dispersion of the harmonic pulse as well as the group veloc-
ity walk-off of the harmonic pulse with respect to the laser
pulse. Both of these effects are negligible for pulses of 100 fs
or longer in a low density (∼ 1019 atoms/cm3 ) gas medium.
To further simplify this equation, we can introduce the
slowly varying spatial envelopes for the harmonic field and
the polarization into (2). These are given by
 Zz 
 
aq (x, t) = Aq (x, t) exp −i qk0 (x, t) + ∆k(x, t) dz 0 ,
−∞
(3)
 Zz 
pq (x, t) = Pq (x, t) exp −i qk0(x, t) dz 0 , (4)
−∞
where k0 is the wave number of the fundamental laser field,
and the phase mismatch of the harmonic with the laser field
is defined as ∆k ≡ kq − qk0. Finally, using the fact that
∂ 2 aq ∂aq
 kq , (5)
∂z 2 ∂z
we arrive at the paraxial wave equation for the qth harmonic:
∂aq 4πω2q
∇⊥
2
aq + 2ikq − 2kq ∆kaq + ikq Nσabs aq = − 2 pq .
∂z c
(6)
To derive this we have explicitly separated the real and imag-
inary part of the harmonic wave number, where kq is the

real part of the harmonic wave number, σabs is the absorption
cross section for harmonic photons, and N is the gas density.
In deriving (6) we have ignored all terms that vary as ∇⊥ kq ;
this is equivalent to saying that ∂n q /∂x = ∂n q /∂y ≈ 0. In do-
ing this we have ignored any refraction of the harmonic field
by a spatially varying refractive index arising from the plas-
ma formation. This is a very good approximation since short
wavelength radiation will be very resistant to refraction by
plasmas because of the large critical density associated with
soft X-ray radiation. The refractive index of a low density
plasma is
1 ne
nq ≈ 1 − , (7)
2 n crit
where n crit is the critical density (the density at which the
plasma frequency equals the laser frequency) and n e is the
electron density. For harmonics with wavelength < 1000 Å,
n crit > 1023 cm−3 , while the average gas density is typically
< 1019 cm−3 in most harmonic experiments. Thus n q ≈ 1 and
the radiation is very insensitive to radial variations in elec-
tron density; n crit for the laser, however, is ∼ 1021 cm−3 . Thus
the radially varying phase imparted to the laser light may not
be negligible and refraction may have an effect on the spatial
profile of the laser [43]. Because the phase of the laser is then
imparted to the harmonic through pq , the far-field profile and
divergence of the harmonics can be affected.
The nonlinear polarization, pq , is the term that drives the
harmonic field. The amplitude of the nonlinear polarization
is proportional to the nonlinear dipole moment of the atoms
in the medium oscillating at the harmonic frequency times
the density of the atoms in the medium. At low intensity, the
phase of the polarization will generally be q times the phase
of the laser. At higher intensity, the phase of the polariza-
tion will be intensity dependent. If we explicitly separate the
intensity dependence of the polarization from the traditional
geometric phase, however, we can write the following for the
nonlinear polarization:
315
with an intensity distribution given as
" #
1 2(x 2 + y2 )
I(x, t) = I0 exp − 2
1 + 4z 2/k02 w40 w0 (1 + 4z 2/k02 w40 )


× exp −4 ln 2t 2 /τFWHM
2
, (9)
(where w0 is the 1/e2 radius of the laser at focus), this phase
is

2k0 (x 2 + y2 )z
ϕGaus(x) = − tan−1 2z/k0 w20 − 2 4 . (10)
k0 w0 + 4z 2
Finally we have included a third contribution to the phase,
ϕran (x, t), which accounts for randomly varying temporal
phase initially on the laser beam. It is this rapidly varying
phase that accounts for imperfect coherence of the laser beam
and may subsequently degrade the coherence of the harmon-
ic.
In the tight focusing limit, namely, that case when the
laser confocal parameter is smaller then the length of the
medium, the geometric phase is very important. It is usually
the limit on the conversion efficiency. The origin of this can
be seen in (10) because the phase of the harmonics produced
on one side of the focus have a phase nearly 180◦ different
from those produced on the other side of the focus (due to
the tan−1 term) and consequently destructively interfere. This
phase can give rise to rings in the harmonics’ far-field pro-
files from geometric phase interferences. However, because
of the much greater conversion efficiency when the laser is
weakly focused (kw20  l), most experiments are conduct-
ed in a regime where geometric phase effects are minimized
and it is the intensity dependent phase and the production
of free electrons that are most important in controlling the
harmonics’ spatial properties.
In addition to the phase contributions outlined above,
examination of (6) indicates that the value of the phase mis-
match ∆k contributes to the harmonics’ phase. Though there
is some phase mismatch associated with the refractive in-
dex of the neutral medium, a much greater contribution to
the phase mismatch is the production of free electrons by the
   laser field during the harmonic generation. Using (7) for the
pq (x, t) ∼
= 2N(x, t) dq [I(x, t)] exp iϕdip [I(x, t)]
 refractive index of the fields in a plasma, this phase mismatch
× exp iq[ϕGaus (x) + ϕran(x, t)] , (8)
where |dq [I(x, t)]| is the amplitude of the intensity dependent
dipole moment oscillating at a frequency q. This dipole has
been calculated numerically from the Schrödinger equation
by a number of groups [18, 44]. In a perturbative treatment it
is simply proportional to the qth power of the laser intensity,
but, in strong laser fields its dependence with laser intensity is
usually slower than this [2].
In (8), we have explicitly written the three different pos-
sible contributions to the phase of the nonlinear polarization,
can be written (when q  1)
∆k ≈ (πq/λ0 )(n e /n crit ) , (11)
where n crit is the plasma critical density at the laser wave-
length. The importance of this term can be simply seen if we
find the solution of (6) in the plane wave limit. (This limit is
a good approximation if the laser is weakly focused through
the harmonic generating medium.) In this limit, ignoring the
geometric phase mismatch and the absorption cross section,
the qth harmonic field exiting a uniform medium of length l
is
as it is these terms that have the greatest effects on the har-  
monics’ profiles and coherence. ϕdip [I(x, t)] is the intensity Aq (t) ∼
dependence of the phase of the dipole, dq [I(x, t)]. This term
has been shown to be very important in shaping the harmon-
ics’ far-field profiles and may be important in a determination
of their coherence [45, 46]; ϕGaus(x) is the phase associated
with a focused laser beam. For a focused Gaussian laser beam
= −2iπkq n 0l dq [A0 (x, t)] eiϕd sinc(∆kl/2)ei∆kl/2 .
(12)
From this expression it is clear that the production of free
electrons not only limits the conversion efficiency through the
sinc term but also imparts phase on the harmonics. This phase
316

can alter the far-field profile [47]. Furthermore, if the time his-
tory of the production of free electrons is not uniform across
the beam, a degradation of spatial coherence can result.
2 Measurements of high-harmonic far field spatial
profiles
the focus. At any time there is a radial intensity profile, which
means that the harmonics are emitted with different phases at
different radial locations. The interference of the different ra-
dial locations causes the harmonic emission to be spread over
a larger angular region than predicted by perturbation theory.

A number of experiments have been conducted to investi-

gate the spatial profiles of the harmonics [33–35]. In general
these experiments produced harmonics by focusing a laser
into the output of a gas jet or a flowing gas medium. Har-
monics produced in the medium are spectrally dispersed in
one dimension with a reflective or transmission grating and
the spatial profiles were measured in the direction perpen-
dicular to the spectral dispersion. This arrangement permits
simultaneous measurement of the spatial profiles on a range
of harmonics.
Tisch et al. reported a measurement of the profiles
from harmonics produced by a 1054 nm, 1 ps, Nd:glass
laser focused into low-density helium at intensities up to
3 × 1014 W/cm2 [33]. This experiment examined harmonics
as high as the 119th order (88 Å). Raw data from that ex-
periment are shown in Fig. 1a. Harmonics of increasing order
are produced toward the right side of these data. In general
this experiment found that the divergence of the harmon-
ic radiation decreased with increasing harmonic order. The
overall divergence of the harmonics tended to be larger then
the perturbation theory prediction for harmonics produced in
an unionized medium [i.e., when Iq (x) ∝ I0 (x)q ].
In addition, the harmonics in the plateau exhibited sub-
stantial structure. Figure 1b shows the lineout of the 71st har-
monic. The harmonic exhibits a smooth central feature that is
surrounded by sharp spikes. This behavior was attributed to
the phase imparted to the harmonic beam by the production
of free electrons. As the gas is ionized by the high intensi-
ty pulse, n e increases resulting in a commensurate increase in
∆k. Because the ionization history varies radially in the fo- a
cus, the exp{i∆kl/2} term imparts a rapidly varying radially
phase that translates to structure in the far field.
Experiments of Peatross et al. also observed structure in
the lower-order harmonics produced in gases of very low den-
sity [35, 45]. These experiments were conducted using a 1 ps
Nd:glass laser focused into a low-density tubular target con-
taining gas. The experiments were conducted in a density
regime in which free electron phase matching effects were
expected to be negligible.
Figure 2 shows the measured far-field pattern of the 11th
through 17th harmonics generated in 0.3 torr of Xe at an in-
tensity of 5 × 1013 W/cm2 [45]. The smooth, solid line shows
the angular pattern of the f/70 incident 1 µm laser. These
profiles are typical of those generated in that experiment, with
a narrow central feature and broad wings or shoulders. The
width of the central feature is consistent with that predicted
from a perturbative calculation where the order of the har-
monic production is of order 5. This is typical of calculations
of high-order harmonic generation [2]. Because of the low gas
density, good focal quality, and large f number (thin target) b
used in these experiments, the only apparent explanation of
Fig. 1. a Spatial profiles from harmonics produced by a 1054 nm,
the wing structure observed was the effect of the phase of the 1 ps, Nd:glass laser focused into low density helium at an intensity of
atomic dipole response to the driving field. For a thin target, 3 × 1014 W/cm2 (taken from [33]). b Lineout of the 71st harmonic from
the emission can be considered to come from a single plane at (a). The dashed line is the prediction of lowest-order perturbation theory

Fig. 2. Spatial profiles from harmonics produced by a 1054 nm, 1 ps,
Nd:glass laser focused into 0.3 torr of xenon at an intensity of 5 × 1013 W/
cm2 (taken from [35])
The spatial profiles from a 100 fs laser have been stud-
ied by Salières et al. [34, 48]. These experiments utilized
a 825 nm, 140 fs Cr:LiSrAlF6 laser focused with an f/25
lens into an argon or neon gas jet. These studies were con-
ducted in gas at higher density then the studies of [33]
and [35]. These experiments found that at low intensity,
namely, that below the ionization saturation intensity (Isat ),
the harmonics exhibited very smooth, single mode Gaus-
sian profiles. (The saturation intensity is the peak inten-
sity at which the ionization rate integrated over the laser
pulse is approximately two, i.e., when nearly 90% of the
atoms have been ionized by the end of the laser pulse.)
Figure 3a shows data taken in Ne under these conditions.
Once again, the harmonics are spectrally dispersed in one
axis and spatially resolved in the other. This data illustrates
that all the harmonics exhibit reasonably smooth profiles
and that the divergence decreases with increasing order. Fig-
ure 3b shows lineouts of selected harmonics. These harmon-
ics exhibit a divergence of roughly 10–20 mrad. This is ap-
proximately the divergence predicted by perturbation theo-
ry.
At higher density and peak laser intensity above the ion-
ization threshold of the gas, the smooth single mode spatial
profiles of the harmonics is no longer preserved [49]. This is
largely due to the refraction of the fundamental beam. This re-
fraction imparts phase distortion on the fundamental, which
is transferred to the harmonic through (8). This effect is illus-
trated in Fig. 4 in which the profiles of harmonics produced
in argon at intensities corresponding to ∼ Isat (Fig. 4a) and
an intensity ∼ 2 × Isat (Fig. 4b) are compared. In these im-
ages, the spectra are dispersed horizontally and the spatial
distribution is in the vertical direction. The images are of the
19th through the 29th harmonic and were taken 75 cm from
317
b
Fig. 3. a Spatial profiles from harmonics produced by a 825 nm,
140 fs, Cr:LiSrAlF6 laser focused into a Ne gas jet at an intensity of
5 × 1014 W/cm2 (taken from [34]). b Lineouts of the 29th, 35th, and 41st
harmonics from (a)
the laser focus. At the lower intensity the profiles are very
smooth and nearly Gaussian. However, at the higher intensi-
ty, the profiles exhibit some breakup from the refraction of the
laser.
Even more dramatic is a consideration of the two-
dimensional images of the harmonics from a refracted laser
beam. Figure 5 shows the images of harmonics produced
from a frequency doubled Nd:glass (526 nm) laser in a heli-
um jet focused with an f/50 lens. These images were taken
on the laser axis with an X-ray CCD detector. The detector
was located 250 cm from the laser focus. A 7500 Å thick alu-
minum filter blocked the laser light and passed the soft X-ray
radiation. The images are essentially a sum of the harmon-
ic profiles of the harmonics that fall between the roll-over of
the CCD detector on the long wavelength side at ∼ 350 Å
and the cutoff of the aluminum filter at 173 Å on the short
wavelength side (i.e., the 15th through the 31st harmonics.)
The first image is of harmonics produced at 2 × 1015 W/cm2
(i.e., ∼ Isat ) the second and third images are at intensities
of 5 × 1015 W/cm2 and 8 × 1015 W/cm2 , respectively (i.e.,
> Isat ). The harmonics exhibit a clean, single mode Gaussian
318
a preserved; however, an interferometric based measurement is
b The coherence of any light field can usually be quantified by
Fig. 4. a Spatial profiles from harmonics produced by a 825 nm, 140 fs,
Cr:LiSrAlF6 laser focused into an Ar gas jet of density ∼ 5 × 1018 cm−3 at
an intensity of 4 × 1014 W/cm2 . b Spatial profiles of harmonics produced
in Ar when the peak intensity is increased to 1 × 1015 W/cm2
a b c Note that Γii (0) is the intensity of the light source at point Pi .
Fig. 5a–c. Images of harmonics in the 173 Å to 350 Å range produced from
a frequency doubled Nd:glass (526 nm) laser in a helium jet focused with
an f/50 lens at an intensity of (a) 2 × 1015 W/cm2 , (b) 4 × 1015 W/cm2 ,
and (c) 8 × 1015 W/cm2
shape at the lower intensity but exhibit severe distortion at
higher intensities.
It is this refraction that sets an upper limit on the use-
ful conversion efficiency that is achievable with high-order
harmonic radiation [49]. Though the harmonic yield scales
as the square of the gas density, implying that increasing the
density is advantageous in achieving high yield, increasing
the density and the laser intensity begins to cause a degra-
dation in the harmonics’ profiles. This may be of concern
for some applications. Equation (7) suggests that higher elec-
tron densities can be tolerated for a short wavelength laser.
Therefore, the refraction effects will be more severe for the
fundamental of a near IR laser at 800 or 1000 nm than for
their second harmonic. This plasma induced phase can also
cause a degradation of the harmonics coherence.
3 Spatial coherence of harmonic radiation
Though the spatial profile studies presented in the previous
section have been very important in unraveling much of the
physics controlling the harmonic generation process, as men-
tioned earlier, they do not contain all pertinent information
about the spatial properties. Of equal importance is the spa-
tial coherence of the harmonic beam, or in other words how
well two parts of the harmonic profile interfere with each
other. The smooth, single mode character of the harmonics
implies that the good coherence of the laser beam is probably
required to quantify it. Because of the more difficult nature of
such experiments, until recently no data existed to help quan-
tify the spatial coherence of the harmonics in the XUV and
soft X-ray region [36].
The simplest interferometric measurement possible is the
well-known Young’s two slit experiment. Before we discuss
the physics affecting the coherence of the harmonics, it is use-
ful to briefly review the mathematics of spatial coherence and
place that in the context of a two-slit experiment.
3.1 Mathematical treatment of coherence
the mutual coherence function [50]. This function is defined
as
Γ12 = a(P1 , t + τ)a∗ (P2 , t) , (13)
where a is the complex electric field amplitude of the field
at points P1 and P2 . The brackets denote an ensemble aver-
age. For all light fields we are concerned with, the ensemble
average can be taken to mean a time average over some ap-
propriate time interval. For an ultrashort pulse, such as a har-
monic, this time interval will almost always be the entire
pulse width [51]. The mutual coherence function is essential-
ly the correlation function between two points in the field of
the light source delayed with respect to each other by a time t.
It is usually convenient to work with the normalized quantity
usually called the complex degree of coherence, which is
Γ12 (τ)
γ12 (τ) = √ , (14)
Γ11 (0)Γ22 (0)
where γ satisfies the relation
0 ≤ |γ12(τ)| ≤ 1 . (15)
If γ is one, the field exhibits complete correlation between the
points 1 and 2 at time delay of t and is said to be fully co-
herent. We are most concerned with the coherence of the field
with no delay between the two points. We will consequently
refer to the complex coherence factor (CCF)
µ12 = γ12 (0) . (16)
Next, we need to relate these quantities to the experimen-
tal setup, namely, the two-slit interference. The experimental
configuration is generically shown in Fig. 6. We will assume
that the slits are very narrow compared to the harmonic beam

Fig. 6. Generic experimental configuration of the Young’s two-slit experi-
ment to measure spatial coherence
so that effectively only one point on the beam is sampled. If
a(P) is the harmonic field at the slit mask, then the harmonic
field at the detector plane, Q, will be
a(Q, t) = K 1 a(P1 , t − r1 /c) + K 2 a(P2 , t − r2 /c) ,
where the K i are constant amplitude factors, which depend on
the diffraction of the field from each slit. We note that the har-
monic intensity detected if light passes through only one slit
will be
319
results from the introduction of a slit pair in the harmonics
beam.
From a practical standpoint, no slits used in any experi-
ment are infinitely thin. They must simply be thin enough to
assure that the diffraction from each slit is sufficient to assure
complete overlap of both diffracted patterns at the detector. In
practice this requires that the xz slit width, D, is D  λz/∆x.
For partially coherent light, it will be useful to compare
the measured dependence of the complex coherence factor
with a known case. It is well known that an extended source of
light, emitting incoherently over its surface, will exhibit some
level of partial spatial coherence when the coherence is meas-
ured a distance z from the source. The complex coherence
factor of an incoherent source can be quite easily calculated
using the well-known van Cittert–Zernike theorem [51]. This
theorem states that the CCF of an incoherent source with an
intensity function I(x) is given, far from the source as
RR  
I(ξ, η) exp i 2π
λz (∆x ξ + ∆y η) dξ dη
µ(x 1 ,y1 ; x 2,y2 ) = RR ,
I(ξ, η) dξ dη
(23)
where ξ and η are the spatial coordinates at the source. This
(17)
result, very similar to the result for Fraunhofer diffraction, in-
dicates that the CCF is simply the Fourier transform of the
source function. For a uniform, circular disk with radius a, the
CCF measured between two points separated by ∆x and ∆y
is
D 2 E  p 
I j (Q) = |K j |2 a (Pj , t − r j /c) . (18)   J1 2πaλz ∆x 2 + ∆y2
µ(∆x, ∆y) = 2 p , (24)
2πa
λz ∆x 2 + ∆y2
Consequently, the intensity detected when both slits are illu-
minated is where J1 (ζ) is the Bessel function of the first kind, order 1.
  
(1) (2) r2 − r1 We can further quantify the coherence of a light source
I(Q) = I (Q) + I (Q) + 2K 1 K 2 Re Γ12 . through the definition of its coherence area. The coherence
c
(19) area is defined as [51]
ZZ
 
Examining (14), we note that the complex degree of coher- Ac = µ(∆x, ∆y) d∆x d∆y . (25)
ence can always be written as γ12 (τ) = |γ12 |(τ) exp[−iωq τ −
iϕ(τ)]. Thus we see that the intensity observed, given by (19),
of course oscillates as r1 −r2 varies. If the detector is far from An incoherent disk of diameter d will have a coherence area
the slits, then the fringes have a spatial period, L, of of Ac = 4λ2 z 2 /πd 2 measured at a distance z from the source.

λr
L= . (20) 3.2 Factors affecting the coherence of the harmonics
∆x
If we then define the fringe visibility on the basis of the max- With these mathematical preliminaries in mind, we are in
imum and the minimum intensities of this intensity pattern a position to consider the factors that can degrade the co-
as herence of the harmonics. We point out initially that if the
Imax − Imin fundamental laser is beam is completely coherent, in the ab-
V= (21) sence of any phase variations imparted on the harmonic, the
Imax + Imin harmonics will also exhibit full coherence. Their phase is
(where Imax and Imin the maximum and minimum intensities simply q times the phase of the laser; so, if the laser phase
of the fringe pattern), then the fringe visibility at the center of is completely correlated over all space, the harmonic’s phase
the pattern is simply will also exhibit complete correlation.
√ However, as we have seen there are a number of factors
2 I (1) I (2) that alter the phase of the harmonics during their generation.
V = (1) γ12 (0) . (22) If these factors impart a time-varying phase that differs from
I + I (2)
one point on the laser beam to the next, then the normalized
We can therefore obtain a direct measurement of the complex time averaged correlation of (14) is less than one. There are
coherence factor by a measurement of the fringe visibility that a couple of factors that can do this.
320

First, from (8), we see that the harmonic has a phase as- If the linearly increasing electron density between points x1
sociated with the intensity dependent dipole. If the intensity and x2 differs by the amount δn e at the end of the pulse, the
at two points on the laser beam are equal, then the time his- electron density can be written
tory of the dipole phase will be the same at these two points. (
If the CCF is then calculated between these two points the (n e0 + δn e ) τtp , i = 1
n e (t) =
i
(27)
phases will cancel and the coherence is not affected. On the n e0 τtp , i = 2
other hand, if the peak intensities differ slightly, the phase his-
tories at the two points on the beam in question will not be and the complex coherence factor is
exactly the same. This will give rise to interference in the time    
integral of (13) and may cause a decrease in coherence. πql t
µ12 = exp −i δn e . (28)
By this reasoning, we note that if the two-slit experiment 2λ0 n crit τp
is performed on the harmonic beam with the slits placed sym-
metrically about the beam center and the laser beam intensi- Time integration yields for the absolute value of the CCF:
ty is radially symmetric, we expect that the fringe visibility   
 πql 
will not be degraded. On the other hand, if the dipole phase
does exhibit significant variation with intensity, as conjec-
tured in [46] and [45], the CCF measured on two points not
radially symmetric will exhibit a decrease in the CCF from
unity as a result of the differing time histories of the phase.
Another contribution to the phase of the harmonics is the
∆k term as manifested in (12). As already discussed, this term
is largely due to the production of free electrons by ionization
when the laser intensity is sufficiently high. Thus, if there are
any density fluctuations or fluctuations in the ionization time
history between two points, the time history of n e , and conse-
quently ∆k will differ. This will also result in a decrease in the
CCF upon time integration in (13). This physics is illustrat-
ed schematically in Fig. 7. Consider two points on the beam
generated by equal peak intensities. If there is a slight densi-
ty difference between the two points, the time history of the
electron density will differ slightly, as shown in Fig. 7. This
electron density time history translates into a phase time his-
tory. The phases between the two points do not cancel and
will affect the time average correlation integral.
We can further quantify this effect by making a estimation
for the harmonic pulse shape. We can derive a simple scal-
ing for the complex coherence factor if we assume that the
harmonic pulse is square in time and that the electron densi-
ty ramps up linearly over the harmonic pulse. In this case, we
approximate the harmonic pulse as
Aq (xi , t) = Aq0 exp{−i∆kl/2}
 
πqn ie (t)
= Aq0 exp −i l , 0 ≤ t ≤ τp ,
2λ0 n crit
1 
|µ12 | = sinc δn e  . (29)
4λ0 n crit
The maximum electron density at which harmonics will be
produced is that at which ∆kl ∼ 2π, implying a maximum
electron density of approximately 1–5 × 1017 cm−3 for the
harmonics in the 500–100 Å range. It is reasonable, therefore,
to assume that the electron density can fluctuate by an amount
that is comparable to this value. Equation (29) implies that
electron density variations of this magnitude will degrade the
coherence to µ ∼ 0.9–0.6, a significant decrease in harmonic
coherence. Equation (29) also implies that the coherence will
be further degraded as q increases.
This coherence degradation by the creation of free elec-
trons is not due to the phase fluctuations imparted directly on
the harmonic by refractive index changes, fluctuations that are
very small for short wavelength harmonic light in low densi-
ty plasma, but is due to the phase fluctuations placed on the
laser beam, which are then transferred to the harmonic. Be-
cause the phase of the harmonic is q times that of the laser’s,
for high orders, it is possible for a very small degradation in
the laser’s coherence to result in a sizable degradation on the
harmonic. This is a general statement, independent of the ac-
tual mechanism by which the laser’s coherence is originally
altered.
This fact can be simply illustrated if we consider two
points on a laser beam with small phase fluctuations between
them. The laser field at the two points 1 and 2 can be written:
 
A1,2 = E 0 (t) exp iωt − ikx + iϕ1,2 (t) , (30)
(26)
which means that the CCF of the laser is
hA1 A∗2 i
µ1,2 (ω) = p
|A |2 |A2 |2
= exp i(ϕ1 − ϕ2 ) , (31)
Zτp
 
= τp−1 exp i(ϕ1 − ϕ2) dt , (32)
0
for a square pulse, where we have simply averaged over the
laser pulse. (τp is the laser pulse width). Since we assume that
the phase fluctuations are small, we can say that the absolute
value of the CCF can be approximated as
Zτp
Fig. 7. General explanation of how a variation in density across the laser  
beam can affect the harmonic’s spatial coherence. If the density between µ12 (ω) ≈ 1 − 1 τ −1 ∆ϕ dt . (33)
2 p
two points in the beam is slightly different, as the medium is ionized, the
electron density will follow the thick solid and dashed curves 0
 321

The harmonic field generated by this laser beam at points 1 the pulses to their original pulse width of 2 ps. The result-
and 2 will be approximately ing pulse energy produced is up to 0.5 J. The beam profile
  after recompression is near Gaussian with a 1/ e2 diameter of
A1,2(q) = E q (t) exp iqωt − iqkx + iqϕ1,2 (t) , (34) 35 mm.
The laser pulses were then frequency doubled in a 1 cm
which means, by the same reasoning, that the magnitude of thick KDP crystal to a wavelength of 526 nm with a con-
the harmonic’s CCF is version efficiency of ∼ 45%. The high-order harmonics were
Zτp produced with 526 nm light instead of 1053 nm light because
  the shorter wavelength drive has been shown to yield high-
µ12 (qω) ≈ 1 − q τ −1 ∆ϕ dt . (35)
2 p er conversion efficiency into harmonics in the 200–500 Å
0 range [23]. As discussed above, it is also expected to be less
susceptible to free electron phase fluctuations. Furthermore,
(now assuming that q∆ϕ is small, which is equivalent to say- the shorter wavelength laser light is also less susceptible to
ing that the laser’s CCF is very close to one). So we see that ionization induced refraction effects within the gas medium.
the CCF of the harmonic and the laser are related by The Gaussian laser beam spatial profile was apertured to
   
a diameter of 1.5 cm immediately prior to the focusing lens
µ12 (qω) ≈ 1 − q 1 − µ12 (ω) . (36)
Thus the deviation of the harmonics CCF from unity will be q
times larger than that of the laser. This reasoning implies that
from the standpoint of preserving the inherent high coherence
of the laser in harmonic generation, it may be advantageous
to use short wavelength laser light to reach short wavelength
harmonics since q can be kept small.
4 Measurement of high-order harmonic spatial
coherence
4.1 Experimental Details
To measure the coherence of XUV radiation produced by
high-order harmonic generation, we executed a Young’s two-
slit experiment. The experimental configuration is shown in
Fig. 8. The majority of the data described in the sections that
follow were of harmonics generated in helium gas. This gas
was chosen because the harmonics produced reach to higher
order and shorter wavelength then the other gases, a feature
essentially due to the high ionization potential of helium. Ex-
periments were also performed in other gases with similar
results.
In our experiment, harmonics were generated with a Nd:
glass laser based on the well-known technique of chirped
pulse amplification. In brief, the laser consists of a diode
pumped, additive pulse mode-locked Nd:YLF oscillator,
whose 1053 nm, 2 ps pulses are stretched to 500 ps with
a dispersive grating/lens stretcher. These pulses are ampli-
fied in a Nd:glass regenerative amplifier and three additional
amplifiers to an energy of 1 J. A grating pair recompresses
to produce a uniform, near flattop profile. This beam was
then focused with a 75 cm focal length, plano-convex lens.
The focal spot of the laser light was measured to be a di-
ameter of 70 µm, indicating that it is very near the diffrac-
tion limit. The laser pulses were focused into a gas plume
produced by a pulsed gas jet that could be backed with up
to 50 bar of pressure (yielding an estimated gas density of
5 × 1018 cm−3 [52]). The high-order harmonics produced in
the 200 Å to 500 Å range were detected with a flat-field soft
X-ray spectrometer located on the laser axis. This spectrom-
eter utilized a horizontal 50 µm entrance slit. The harmonic
radiation was dispersed with a flat field, grazing incidence,
gold-coated 1200 line/mm grating. The soft X-rays were then
detected with a Cs:I coated, two-stage microchannel plate that
was coupled to a phosphor readout. The signal was then col-
lected with a lens and a CCD camera. The total distance from
harmonic source (laser focus) to the entrance slit was 130 cm
and the distance from source to detector was 180 cm. Because
the grating focuses only in the dispersing direction and does
not alter the divergence of the radiation in the transverse di-
rection, this configuration permits simultaneous measure of
spectral information on one axis, with a measure of the spatial
profile of each harmonic on the transverse axis.
4.2 Raw data
A typical spectrum of harmonic radiation collected with
this configuration is shown in Fig. 9. This spectrum shows
the spatially integrated spectrum of high-order harmon-
ics produced with 526 nm light in He at an intensity of
4 × 1015 W/cm2 . The spectrum exhibits the classic high-
order harmonic behavior, the production of a plateau of
Fig. 8. Experimental configuration used to
measure the high-order harmonics’ spatial co-
herence
322

slits in 20 µm thick Ti foil. Each slit had a width of 8 ± 1 µm

and slit pairs with spacings of 28, 50, 75 and 100 µm were
used for the measurements. Because of the proximity of the
slit pairs to the laser focus (the laser was roughly 1 mm in di-
ameter at the slits), the slits began to show laser damage after
10 to 20 full-power laser shots. To monitor this degradation,
the slits were backlit at a slight angle with a HeNe laser and
the image of the slits was imaged outside the vacuum cham-

Fig. 9. Spatially integrated spectrum of high-order harmonics produced with

526 nm light in He at an intensity of 4 × 1015 W/cm2

Fig. 11. Measured profile of the 13th harmonic at the location of the dou-
ble slits (4 cm from focus) generated at an intensity of 4 × 1015 W/cm2 .
This was measured by scanning a single slit across the harmonic profile.
The solid line is a Gaussian fit to the data

Fig. 10. Angularly resolved spectrum of high-order harmonics produced

with 526 nm light in He at an intensity of 4 × 1015 W/cm2

harmonics to a high order with a sharp cutoff below a cer-

tain wavelength (in this case occurring at the 23rd harmonic
λ ≈ 229 Å). The harmonics produced under these condi-
tions exhibit smooth, low divergence spatial profiles. A two-
dimensional raw image of harmonics produced under the
same conditions as Fig. 9 is shown in Fig. 10. The harmon-
ics are dispersed in the vertical direction; their far-field spatial
profile is manifested in the horizontal profile. These harmon-
ics clearly exhibit smooth, single mode Gaussian far-field
profiles, similar to the results reported in [34].
To measure the spatial coherence, we introduced slit pairs
into the harmonic’s beam before the spectrometer (see Fig. 8)
to generate interference fringe patterns on each harmonic. Be-
cause of the short wavelength of the harmonics, it is necessary
to use open slits to produce the interference fringe pattern.
These slits need to be sufficiently narrow to ensure that only
a small portion of the harmonic beam is sampled by each
slit. Furthermore, we require that each slit be narrow enough
to assure that the diffraction of the beam from each slit is
fast enough to yield complete overlap of the radiation pass-
ing both slits at the detector. This implies that the slits need to
be no wider than 10 µm. On the other hand, the slits must be
wide enough to pass enough radiation for the fringe pattern to
be detectable on each laser shot.
With these considerations, we found that the optimal con-
figuration was to use slit pairs of roughly 8 µm width placed
4 cm from the gas jet plume and laser focus. The slit pairs Fig. 12. CCD image of fringes generated on the 11th to the 19th harmonic
used in the experiment were produced by laser drilling the in helium with a peak intensity of 6 × 1015 W/cm2

ber with magnification. During the experiment when the slit
exhibited some damage, it was replaced by an unused slit foil
in the position of the original slits. The slit pairs were placed
perpendicular to the 50 µm entrance slit of the spectrome-
ter. The total distance from the slit pair to the detector was
176 cm. This distance assured that the harmonic fringe spac-
ing (> 600–1000 µm) was larger than the estimated 100 µm
spatial resolution of the detector.
The profile of the harmonics at the position of the slit pairs
was measured by placing a single 8 µm slit at the same posi-
tion as the slit pairs and scanning the slit across the beam. The
measured profile of the 13th harmonic generated at an intensi-
ty of 4 × 1015 W/cm2 is shown in Fig. 11. This measurement
is characteristic of all of the harmonics, which, in general,
have a diameter of roughly 350 µm.
A typical raw image of a fringe pattern generated in the
configuration of Fig. 8 by a slit pair with a 50 µm spacing
placed in a beam of harmonics is shown in Fig. 12. This is da-
ta of harmonics generated at an intensity of 6 × 1015 W/cm2
in helium. In this image, fringes on all the harmonics (the
11th to the 19th) are clearly visible. All the harmonics exhibit
some coherence under these conditions. From an analysis of
such images it is possible to determine the harmonic fringe
visibility under a variety of conditions.
It is also important to note that the coherence of the laser
used to generate these harmonics is very good. Fig. 13 shows
lineouts of fringes generated by the laser itself. These fringe
Fig. 13. Lineout of fringes generated by the 526 nm laser beam with three
different slit separations. The fringes were generated with the same slit
pairs used for the harmonics in vacuum, 4 cm from the laser focus with the
detector located 200 cm from the slit pairs
323
Fig. 14. Comparison of fringes produced by the laser with a 50 µm slit pair
when the laser propagates only through vacuum at its focus and when the
laser propagates through the ionizing gas jet at focus. Both fringe patterns
were produced when the laser peak intensity at focus was 5 × 1015 W/cm2 .
(The gas jet backing pressure was 50 bar)
patterns were generated with the same slits used for the har-
monics; however the laser beam was reflected out of the
chamber after the slit pairs and detected with a CCD cam-
era. Figure 13 shows the laser fringes in vacuum (no gas jet)
with three slit spacings. The fringe visibility is > 0.9 for all
three slit separation. We also note that propagation of the laser
through the gas jet does not significantly degrade the coher-
ence of the laser. Figure 14 compares the fringe pattern of
the laser generated with 50 µm slit separation when the laser
propagates only in vacuum inside the chamber and the fringe
pattern at the same laser intensity with the gas jet pulsed, so
that the laser has propagated through the harmonic generating
medium. As can be seen in this figure, the laser’s fringes do
not change dramatically upon propagation through the gas jet.
4.3 Coherence measurement results
To derive information about the harmonics mutual coher-
ence function and how it changes with changing parameters,
we have examined the fringe visibility of the harmonics as
a function of a number of parameters. Lineouts of typical in-
terference patterns obtained by using slits with a 50 µm spac-
ing centered on the harmonic beam are shown in Fig. 15. Here
fringe patterns on the 11th to the 19th harmonic are shown
(covering the wavelength range of 277 to 479 Å). These data
were taken with a peak laser intensity of ∼ 4 × 1015 W/cm2 ,
an intensity above the ionization saturation intensity in heli-
um (∼ 1 × 1015 W/cm2 ). As shown above in Fig. 12, all the
harmonics exhibit interference fringes. However, the fringe
visibility is < 1.0, indicating that all the harmonics exhibit
some degree of partial coherence over a separation of 50 µm.
In fact, the fringe visibility decreases with increasing
harmonic order. Figure 16 shows the measured visibility
with a 50 µm slit spacing as a function of harmonic order
from the 11th to the 19th harmonic for two peak intensities:
1 × 1015 W/cm2 and 4 × 1015 W/cm2 . Each point in this fig-
ure represents the average of 6 laser shots within a ±10%
energy bin. The error bars in the measurement were deter-
mined by the extent of the shot to shot variation of the fringe
visibility. At the lowest intensity, the fringe visibility is virtu-
ally constant over the harmonic order considered here, though
324
Fig. 15. Lineouts of typical interference patterns obtained using slits with
a 50 µm spacing centered on the harmonic beam produced with an intensity
of 4 × 1015 W/cm2 and a gas jet backing pressure of 50 bar
Fig. 16. Fringe visibility as a function of harmonic order for two different
peak intensities
there is a slight decrease in visibility as the order increases:
the visibility is 0.6 for the 11th harmonic while it drops to
0.45 for the 19th harmonic. At the higher intensity, however,
the variation of the fringe visibility with increasing harmonic
order is more pronounced, falling faster with increasing order
than the lower intensity harmonics. Here the visibility on the
11th harmonic is 0.45 and the visibility drops to 0.18 on the
19th harmonic.
Figure 16 also indicates that there is a variation in the har-
monic fringe visibility with laser peak intensity. This effect
is illustrated in Fig. 17 where the images and the resulting
lineouts of the fringes from the 11th harmonic (λ = 479 Å)
generated with slits of 50 µm separation are shown at two dif-
ferent peak intensities. In both cases the slits were centered
on the beam. The first image shows the fringes generated
with a peak intensity of 8 × 1014 W/cm2 , below the onset
of significant ionization in the helium gas. Here the fringes
are sharp and well defined with a corresponding visibility
Fig. 17. Images and the resulting lineouts of fringes from the 11th harmonic
(λ = 479 Å) generated with slits of 50 um separation at two different peak
intensities
Fig. 18. Fringe visibility of the 15th harmonic as a function of laser peak
intensity
of 0.8. In contrast, at the higher intensity of 5 × 1015 W/cm2 ,
an intensity at which significant ionization has occurred in
the helium [53], the fringes are broadened, with a drop in
visibility to 0.45.
This trend is reflected over the intensity range from the
mid 1014 W/cm2 to the mid 1015 W/cm2 , the range over
which helium ionization becomes important. Figure 18 illus-
trates the visibility for fringes of the 15th harmonic (λ =
351 Å) with 50 µm spaced slits as a function of intensity. Be-
low the ionization saturation intensity the harmonic exhibits
good fringe visibility of between 0.7 and 0.8. This visibility
falls and levels off at about 0.4 at the highest intensity. The
drop in fringe visibility illustrated here corresponds closely
to the onset of significant ionization [53]. This data also indi-
cates that at low intensity, the coherence of the harmonics can
be quite high, nearly that of the laser itself with the same slit
separation.
One interesting trend of the fringe visibility is illustrated
in Fig. 19. Here is shown the fringe visibility of the 13th har-
monic with a 50 µm slit spacing as a function of the position
of the center of the slit pair across the harmonic beam. The
peak laser intensity is 5 × 1015 W/cm2 , an intensity above
ionization saturation and a regime where the fringe visibili-
ty is degraded. In the center of the beam, the fringe visibility
is 0.4. However, as the slit pair is moved out to larger ra-
dius, the visibility increases. At a radius of 200 µm, near the
edge of the harmonic beam (see Fig. 11), the fringe visibili-
ty has increased to nearly 0.7. This trend is reproduced in all
of the harmonics studied and is also evident when larger slit
spacings are used.
Furthermore, we find that, at the high backing pressures
used in our experiments, the fringe visibility does not sig-
nificantly change with changing backing pressure. Figure 20

Fig. 19. Fringe visibility of the 13th harmonic with a 50 µm slit spacing as
a function of the position of the center of the slit pair across the harmonic
beam. (The peak laser intensity is 5 × 1015 W/cm2 )
Fig. 20. Fringe visibility of the 15th harmonic through a 50 µm slit spacing
at an intensity of 6 × 1015 W/cm2 as a function of jet backing pressure with
the slits centered
shows the fringe visibility of the 15th harmonic through
a 50 µm slit spacing at an intensity of 6 × 1015 W/cm2 as
a function of jet backing pressure with the slits centered. At
these pressures the gas density in the gas jet scales linear-
ly with gas backing pressure, so Fig. 20 essentially shows
the fringe visibility as a function of gas density. The fringe
visibility is roughly constant at a value of around 0.3 over
the pressure range studied. (The decrease in signal at lower
backing pressures precluded an accurate measurement of the
visibility below 6 bar.)
Despite the decrease of coherence with increasing laser
intensity, we find that the spatial coherence of the harmonics
is still high even at the high intensities. It is possible to recon-
struct the complex coherence factor and the effective coher-
ence area of the harmonics by measuring the fringe visibility
as a function of slit spacing. Such measurements at an inten-
sity of 4 × 1015 W/cm2 on the 13th harmonic (λ = 405 Å) are
shown in Fig. 21a. The same measurement on the 19th har-
monic (λ = 277 Å) is shown in Fig. 21b. (Inadequate spatial
325
Fig. 21a,b. Fringe visibility of the 13th harmonic (a) and the 19th harmonic
(b) as a function of slit spacing when the slits are centered on the harmonic
beam. The short dashed lines are the calculation of the CCF as a function
of separation of uniform incoherent disks of 15 and 16 µm diameter, respec-
tively. The long dashed line is the result of a calculation assuming a 65 µm
diameter incoherent disk
resolution prevented an accurate measurement of the visibil-
ity on the 19th harmonic with a 100 µm slit spacing.) From
this measurement (which essentially gives the complex co-
herence factor µ(∆x, ∆y) as a function of spacing ∆x), we
can use (25) to estimate the effective coherence area Ac . If
we assume that the CCF is azimuthally symmetric, we find
that the coherence area of the two beams are 1.5 × 10−4 cm2
and 6.1 × 10−5 cm2 for the 13th and 19th harmonics, respec-
tively. The coherence area can then be related to an effective
incoherent source size using the van Cittert–Zernike theo-
rem. Using the coherence area of a uniform disk, the effective
incoherent source size is
2λz
ds = √ (37)
πAc
Here z is the distance from source to slits. This quantity is,
in other words, the diameter of a uniform, incoherent source,
which yields the same coherence area as that measured. Thus
a smaller effective source size indicates a higher degree of co-
herence. Using this definition, we find that the 13th and 19th
harmonics exhibit roughly similar coherence source sizes.
The 13th harmonic exhibits an effective incoherent source
diameter of 15 µm, while the 19th has a diameter of 16 µm.
For comparison, the modulus of the complex coherence
factor of a uniform incoherent disk emitting radiation at
a wavelength of 405 Å located at the laser focus with a diame-
ter of 15 µm calculated using the van Cittert–Zernike theorem
is plotted on the data for the 13th harmonic and a similar
plot for a 277 Å source with a diameter of 16 µm is com-
pared to the data for the 19th harmonic. Clearly this simple
model gives a reasonable estimation for the observed charac-
ter of the complex coherence factor. The calculated coherence
factor of a 65 µm source is also shown on these data in this
figure; 65 µm is the estimated size of the harmonic emission
exiting the gas medium as calculated by a numerical solution
326
Fig. 22. Fringe pattern on the 9th harmonic produced in Ar with 50 µm slits
with a peak intensity of 1 × 1015 W/cm2
of the wave equation for the 13th harmonic [54]. Our calcula-
tions indicate that the actual harmonic source size is, in fact,
roughly equal to the laser spot source size (∼ 70 µm, 1/e2 di-
ameter) despite the nonlinearity of the harmonic generation
process because the harmonic yield is strongly saturated in
the center of the Gaussian focus profile. The comparison in
Fig. 21 clearly indicates that the observed harmonic’s coher-
ence is significantly better than a purely incoherent 65 µm
source of radiation produced at the laser focus.
Though all the studies presented thus far have been with
harmonics produced in helium, we also note that good co-
herence has been observed on harmonics from other gases as
well. Figure 22 shows the fringe pattern on the 9th harmon-
ic produced in Ar with 50 µm slits under conditions similar to
those of the helium harmonics (Intensity = 1 × 1015 W/cm2 ).
The fringe visibility is very good with µ = 0.8.
5 Discussion of the coherence results
The measured visibility of the harmonics indicates that the
coherence of the harmonics is quite high. However, it is also
clear that it is not perfect, particularly at high intensity. This
is interesting in light of the fact that the laser exhibits near-
ly perfect coherence, even upon passage through the gas jet.
Much of these observations can be explained in the context of
the discussion of Sect. 3.
The most striking trend in the harmonics’ fringe visibil-
ity is the decrease of the visibility with increasing intensity.
The observed partial degradation of coherence at high laser
intensity is, according to the data of Fig. 18, apparently cor-
related with the onset of ionization in the helium. This seems
to indicate that the formation of a plasma by ionization is the
primary cause of the observed decrease in coherence. This
seems to argues for the free electron mechanism discussed in
the context of (29). This model, and the simple scaling re-
lation, are also consistent with the observed decrease in the
visibility with increasing harmonic order. The observed fall of
the CCF from 0.8 to about 0.5 at the highest intensity for the
15th harmonic is completely consistent with the predictions
of (29).
This decrease in coherence is also consistent with the
measured coherence of the laser. As we discussed in Sect. 3,
the deviation of the harmonics CCF will be expected to be
larger then that of the laser by roughly the harmonic order.
Thus the observed harmonic coherence of 0.5 at the highest
intensity would imply that the laser need only have a coher-
ence drop of 0.95, which is within the error of the measure-
ments of Fig. 14.
The electron density fluctuations may be the result of two
factors. First, intensity variations across the laser focus, per-
haps induced by refraction, could cause varying ionization
histories over the harmonic beam. Similarly, density fluctua-
tions in the initial gas density could also give rise to a time-
dependent electron density difference between two points (as
illustrated in Fig. 7).
To further illustrate this point, we have performed numeri-
cal calculations to derive the harmonic field in the presence of
initial gas density variations. This model involves solving the
wave equation for the harmonic field in the presence of ion-
ization and has been described previously in detail [54]. For
illustrative purposes, the calculated complex coherence fac-
tor of the 15th harmonic as it exits the medium as a function
of spacing is shown in Fig. 23 for two intensities. This cal-
culation assumes a 1 ps, 527 nm pulse in 1 mm of helium gas
with a mean density of 5 × 1018 cm−3 . A 30% initial density
ramp is placed across the 70 µm Gaussian focal spot in one
spatial direction. (This density profile is chosen for illustra-
tive purposes only, but it is not unreasonable to assume that
gas density variations of this order can occur across the profile
of the gas jet output at the high backing pressure used in our
experiment [55].) As shown in Fig. 23, with a peak intensity
of 5 × 1014 W/cm2 , the harmonic exhibits near perfect coher-
ence across the beam. At an intensity of 3 × 1015 W/cm2 , the
coherence is clearly degraded.
Though the calculated coherence factor does not exactly
match the observed decrease in coherence, we emphasize that
this calculation is meant only for qualitative estimates. For
example, our model does not include laser beam refraction
and filamentation in the plasma, effects which are, in gener-
al, difficult to model accurately. Nonetheless, it is clear from
this analysis that spatial nonuniformities in the free electron
formation can have a dramatic effect on the spatial coherence
of the harmonics.
Though the fringe visibility does not vary with gas jet
backing pressure, this does not necessarily contradict the hy-
pothesis that free electrons are the cause of the coherence
degradation. Though the background gas density varies as
the backing pressure is changed, it should be noted that the
maximum electron density at which harmonics are produced
is not necessarily determined by this maximum density. As
Fig. 23. Numerically calculated complex coherence factor of the 15th har-
monic as it exits the medium as a function of spacing for two intensities
found by solution of the wave equation for the harmonic. This calculation
assumes a 1 ps, 527 nm pulse in 1 mm of helium gas with a mean density
of 5 × 1018 cm−3 . A 30% initial density ramp is placed across the 70 µm
Gaussian focal spot in one spatial direction

illustrated by (12), the harmonic yield essentially drops to
zero when ∆kl ∼ 2π. This implies that the maximum elec-
tron density at which harmonics will be produced is about
1–5 × 1017 W/cm2 for the 11th to the 19th harmonics. At the
high backing pressures used in our experiments, the average
background density was higher then 1018 cm−3 . As the gas
density is changed, the effective free electron density seen by
the harmonics does not. Thus it is not inconsistent that the
fringe visibility does not change with backing pressure.
As discussed in Sect. 3, the intensity-dependent dipole can
also degrade the coherence. That this is not the dominant
physics is indicated by two factors. First, the decrease in co-
herence seems to be closely correlated with the onset of ion-
ization in the helium. Any effects of the intensity-dependent
dipole will be present in the absence of ionization. Further-
more, if the intensity-dependent dipole were important, we
would also expect that the observed visibility would decrease
with as the slit pair is moved to one side, away from the cen-
tral axis of the laser focus. In fact what is observed is the
opposite of this; the fringe visibility improves as the slits are
moved away from the center of the beam.
The reason for this trend in the data can probably be ex-
plained by the fact that our measurements were performed
with the slit pairs placed a small distance down stream of the
harmonic near field. This situation is illustrated schematically
in Fig. 24. Though the slit pairs are placed within a confocal
parameter of the harmonics from the laser focus, some propa-
gation of the harmonic beam occurs before the slit mask.
When the laser peak intensity is above the ionization thresh-
old, toward the temporal peak of the pulse, no harmonics are
produced in the center of the beam because of the production
of free electrons. As a result, the harmonic emission at a giv-
en time exits the medium as a ring whose thickness is much
smaller than it radius (see [54] for a calculation of this ef-
fect). The radii of these rings increases later in the pulse as
the intensity increases and ionization has occurred at larger
Gas
Fig. 24. Illustration of the physics giving rise to an increased fringe visibili-
ty as slit pairs are moved from the center of the harmonic beam to one side
of the beam
327
and larger radius. This ring is composed of an annulus that
is much smaller then the total diameter of the beam. After
the beam exits the medium, these annuli begin to spread by
diffraction.
When the slits are placed symmetrically about the laser
focus, one slit is illuminated by one side of the ring, while
the other is illuminated by the other side. When the slits are
moved to one side, both slits are illuminated almost com-
pletely by the diffracted light from one side of the annulus.
Thus, when the slits are placed in the center, they essential-
ly compare the coherence of the light produced over a large
distance, namely, the radius of the anulus. However, when
the slits are placed to one side, they effectively sample only
light produced over a very narrow region. As a result, the ob-
served fringe visibility is high toward one side and lower in
the center.
6 Conclusion
In conclusion, we have examined recent results on the spatial
properties of short wavelength high-order harmonic radiation.
The harmonics represent a novel way of generating bright,
coherent soft X-ray radiation. They exhibit smooth, nearly
Gaussian spatial profiles, though they have some structure un-
der certain conditions. In general, there are a number of fac-
tors that can shape the harmonic’s spatial profile. The phase
slip associated with a Gaussian beam can have some effect,
but with weakly focused beams this is usually not a prob-
lem. More significant is the radially varying phase imparted
across the harmonic beam due to the intensity dependence
of the nonlinear polarizability. This has been shown to be
very important in the development of “wings” on the har-
monic profile. Also important are the phase shifts associated
with the free electron production by optical ionization. Not
only do free electrons impart phase to the harmonic beam
but they also cause refraction and breakup of the fundamen-
tal beam, which is manifested in the harmonics’ profiles. We
have also presented the first measurement of the spatial coher-
ence of high-order harmonic radiation in the soft X-ray region
of 270–480 Å. We find that the harmonics exhibit good coher-
ence, even at high intensity, though the coherence is degraded
by the onset of ionization in the medium. The magnitude of
the coherence degradation is consistent with some simple es-
timates and harmonic production calculations in the presence
of density variations. We find that the harmonics exhibit an
effective incoherent source size that is approximately 15 µm
in diameter. The observed trends in the harmonics’ coherence
seem to be consistent with phase fluctuations imparted by
free electron production through ionization. However, there
may be some degradation effects from the phase differences
resulting from the intensity dependent dipole as well. Fu-
ture experiments will have to be conducted to determine the
details shaping the harmonics’ coherence.
Finally we note that the coherence characteristics of the
harmonics are substantially superior to those of previously
reported measurements of X-ray laser coherence, which typ-
ically exhibit an effective coherence source size of ∼ 100 µm
[38]. Thus the coherence area of the harmonics is nearly
two orders of magnitude larger than soft X-ray lasers. These
results confirm that the harmonics are promising for inter-
328
ferometric applications requiring good coherence or high-
intensity applications demanding good, single mode beams.
Acknowledgements. We thank P. Ruthven and A. Gregory for technical as-
sistance. This work was funded by the EPSRC and the Ministry of Defence.
R.A. Smith is supported by an EPSRC fellowship, and D.D. Meyerhofer’s
work is supported by the National Science Foundation and a NATO Collab-
orative Research Grant.
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