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Interaction of High-Intensity Femtosecond Radiation With Gas Cluster Beam:

Effect of Pulse Duration on Joint Terahertz and X-Ray Emission

Article in IEEE Transactions on Terahertz Science and Technology · November 2016

DOI: 10.1109/TTHZ.2016.2617867

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70 IEEE TRANSACTIONS ON TERAHERTZ SCIENCE AND TECHNOLOGY, VOL. 7, NO. 1, JANUARY 2017
Interaction of High-Intensity Femtosecond Radiation
With Gas Cluster Beam: Effect of Pulse Duration
on Joint Terahertz and X-Ray Emission
Alexei V. Balakin, Murat S. Dzhidzhoev, Vyacheslav M. Gordienko, Mikhail N. Esaulkov, Irina A. Zhvaniya,
Konstantin A. Ivanov, Igor A. Kotelnikov, Nikolay A. Kuzechkin, Ilya A. Ozheredov, Vladislav Y. Panchenko,
Andrey B. Savel’ev, Mikhail B. Smirnov, Peter M. Solyankin, and Alexander P. Shkurinov
Abstract—This paper studies the phenomenon of joint genera-
tion of terahertz (THz) and X-ray radiation in the argon nanoclus-
ter jet under the action of high-power femtosecond laser pulse in
both the single-color and dual-color regimes. It was discovered
that in a gas cluster beam the pulse duration affects the proper-
ties of THz and X-ray emission differently. For the same given
total energy of optical pulse in the dual-color excitation regime of
cluster medium, more than a five times increase of THz radiation
power was observed in comparison with the single-color regime,
while the conversion efficiency to the argon X-ray K-line reached
7 × 10−6 and remained unchanged. The possibility of separation
of contributions of different beam components into the THz sig-
nal was demonstrated experimentally, using contributions from
clusters and nonclustered gas as an example. We suggest an in-
terpretation of experimental results based on a theoretical model
of cluster ionization that self-consistently predicts the level and
dynamics of ionization and electron temperature in the clusters.
Index Terms—Femtosecond laser pulses, gas cluster beam/jet,
high-intensity radiation, nanoplasma, quadrupole radiation, tera-
hertz (THz) and X-ray emission.
I. INTRODUCTION
HE interaction of intense laser pulses with clusters
T consisting of atoms and molecules has been the subject
Manuscript received April 25, 2016; accepted October 6, 2016. Date of pub-
lication November 9, 2016; date of current version January 12, 2017. This work
was supported by the Russian Foundation for Basic Research under Grant 14-22-
01098, Grant 14-02-00979 OFI-M, and Grant 16-32-60171, and in part by the
Russian Science Foundation (RSF) under Grant 16-42-01060. (Corresponding
author: Alexander P. Shkurinov.)
A. V. Balakin, M. S. Dzhidzhoev, V. M. Gordienko, I. A. Zhvaniya, K. A.
Ivanov, I. A. Ozheredov, A. B. Savel’ev, P. M. Solyankin, and A. P. Shkuri-
nov are with the Faculty of Physics and International Laser Center, M. V.
Lomonosov Moscow State University, Moscow 119991, Russia (e-mail: a.v.
balakin@physics.msu.ru; djidjoevms@mail.ru; gord@phys.msu.ru; irina.
zhvaniya@physics.msu.ru; iv_konst_an@rambler.ru; ozheredov@physics.
msu.ru; abst@physics.msu.ru; soluankp@yandex.ru; ashkurinov@physics.
msu.ru).
M. N. Esaulkov, N. A. Kuzechkin, and V. Y. Panchenko are with the Institute
on Laser and Information Technologies, Russian Academy of Sciences, Shatura,
Moscow, 140700, Russia (e-mail: esaulkov_mich@mail.ru; lents125@mail.ru;
vpanch@rfbr.ru).
I. A. Kotelnikov is with the Budker Institute of Nuclear Physics,
Novosibirsk State University, Novosibirsk, 630090, Russia (e-mail: igor.
kotelnikov@gmail.com).
M. B. Smirnov is with the National Research Center “Kurchatov Institute,”
Moscow, 123182, Russia (e-mail:mbsmirnov@gmail.com).
Color versions of one or more of the figures in this paper are available online
at http://ieeexplore.ieee.org.
Digital Object Identifier 10.1109/TTHZ.2016.2617867
2156-342X © 2016 IEEE. Personal use is permitted, but republication/redistribution requires IEEE permission.
See http://www.ieee.org/publications standards/publications/rights/index.html for more information.
of intensive studies in the last two decades [1]–[10]. Clusters in
a supersonic jet, obtained by the adiabatic condensation of gas
flow expanding through a nozzle into evacuated chamber [11]–
[13], combine the advantages of both solid-state and gas matter.
Indeed, first experiments on cluster irradiation by laser pulses
revealed considerable difference in properties of excited matter
consisting of clusters in relation to that consisting of gas atoms.
Various nonlinear effects were predicted and later observed
in the process of interaction of intense femtosecond laser pulses
with cluster beams. These effects include generation of optical
harmonics [5] and self-focusing [6]. It was also shown that the
absorption of laser radiation in a cluster beam could reach a
high value (up to 95%) because of linear (Mie) and nonlinear
resonance interactions [14], [15].
One of the most exciting effects that was observed in cluster
matter was the emission of powerful X-ray pulse [3], [4], [16],
[17]. Later this effect was phenomenologically explained in
[18] and [19] using the following arguments. Atoms, which
constitute the clusters, are multiply ionized under the impact
of laser pulse. As a result, the cluster turns into plasma with
the solid density. Due to high local density in the cluster which
exceeds gas density by three orders, some part of ions gets
excited as a result of electron–ion collisions and emits X-ray
quants. In a gas medium, the probability of ion excitation is low
due to its low density. It also has to be noted that the charge
of ions in the cluster is higher than in an ordinary gas medium.
Thus, the dramatic increase of X-ray intensity is caused by the
presence of clusters; and this effect can be used for preliminary
testing for their presence in the target.
At first sight, it seems that there is no need to carry out joint
measurements of X-ray and THz spectra in cluster medium.
However, some aspects of this problem deserve attention. The
generation of THz radiation in a single cluster and in a cluster
beam is a new phenomenon, which has not been studied yet.
The X-ray, which appears in the beam, could be used as an
additional diagnostic tool in order to investigate such specific
properties as local density and plasma temperature inside the
filament. The generation of X-ray radiation in cluster medium
is thoroughly studied, especially in the most recent works [20].
The sequence of processes causing it is known: the ionization
of atoms affected by the influence of laser pulse, followed by
the excitation of multicharged ions in the cluster resulting from
BALAKIN et al.: INTERACTION OF HIGH-INTENSITY FEMTOSECOND RADIATION WITH GAS CLUSTER BEAM
nonelastic electron collisions (including the ones by means of di-
electronic recombination and photorecombination) at the initial
stage of nanoplasma existence and further X-ray quant emission
[19], [20].
Studies of generation of THz radiation in the cluster medium
are gaining momentum [21]. There are a number of experiments
confirming high efficiency of THz generation. Recently, the
intense THz generation in an argon cluster beam excited by
femtosecond laser pulses was reported in [8]–[10]. Nagashima
et al. [8], [9] observed more than two orders of magnitude
enhancement in total THz pulse energy from argon cluster beam
compared to that from gaseous argon, at equal average atomic
density. In [9] and [10], Jahangiri et al. reported that the spatial
distribution of emitted THz radiation from a cluster plasma has
a four-lobed structure. Unfortunately, up to now there has been
no clear theoretical interpretation of the experimental results
or complete understanding of the mechanism of low-frequency
THz emission from cluster plasma irradiated with high-intensity
femtosecond optical pulses.
Jahangiri et al. [9], [10] also stated that THz pulse energy
dependence on laser energy demonstrates nonlinear growth ac-
cording to “square law” without any saturation, at least, up to
70 mJ per laser pulse (that was a maximum available value
of femtosecond pulse energy in the experiments, which corre-
sponds to the vacuum intensity ∼ 1017 W/cm2 ). Jahangiri et al.
[10] suggested that this low-frequency radiation originates from
time-varying electrical quadrupoles produced by charge separa-
tion due to ponderomotive force.
A way to increase the efficiency of optical-to-THz conver-
sion in a laser-induced plasma of gas medium was success-
fully demonstrated in [22]: The fundamental frequency of Ti-
Sapphire laser was mixed with its second harmonic for the
generation of intense ultrafast THz pulses by four-wave rec-
tification. This led to the increase of the THz yield by 2–3
orders of magnitude as compared with a single-color excitation
regime (fundamental frequency ω only). In spite of the fact that
nowadays the dual-color scheme is widely used for efficient
THz generation in gas media, the efficiency of optical-to-THz
conversion in laser-induced plasma of gas medium even under
dual-color excitation regime is still low [23].
There is a special reason for the use of jets for high-power
THz generation. At high intensity of laser radiation, the bulk gas
plasma becomes so dense that it leads to the absorption of THz
radiation, which is demonstrated in the saturation of THz yield
[24]. It is expected that the transition from the bulk medium to
the gas and cluster jets offers the solution to this problem.
The study of the intense laser pulses interaction with the clus-
ter beams seem quite attractive because its results are in demand
for a variety of applications including practical development of
effective sources of pulsed THz and X-ray radiation. It is also
worth mentioning that the joint use of X-ray and THz radiation
enables more complete research of the matter as the results of
such studies complement each other.
In this paper, we present the results of experimental study
of the generation of THz radiation in the laser-induced clus-
ter plasma. We have performed experiments using both single-
color and dual-color excitation schemes. Simultaneously with
71
the control of THz emission from cluster plasma, we measured
the power and the spectrum of the accompanying X-ray radi-
ation, which is an important source of information about the
processes that occur in cluster plasma [20]. The experimental
results are supported by the theoretical interpretation.
II. EXPERIMENTAL SETUP
The experimental setup was elaborated for the study of the
interaction of high-intensity ultrashort laser pulses with atomic
clusters. It combines three main modules: a source of ultrashort
high-energy optical pulses, a cluster production module, and a
system of THz and X-ray radiation detection. As the source of
optical radiation, we used CPA laser system based on a fem-
tosecond Ti:Sapphire laser with multipass amplifier. Our laser
system provides pulses with energy up to 30 mJ at repetition
rate of 10 Hz, 810-nm central wavelength, beam diameter of
1.5 cm, and quality factor M 2 = 1.6. Pulse duration τ is tuned
in the range of 50–600 fs by chirping the laser pulse in a vacuum
grating compressor.
For the cluster production, we applied the technique of adia-
batic expansion of the gas into vacuum through a special nozzle
[11]–[13]. We used a supersonic conical nozzle with input diam-
eter din = 0.7 mm, output diameter dout = 4.7 mm, half opening
angle α = 5◦ , and 24.7 mm length. The nozzle is connected to
a high-pressure chamber with a pulsed electromagnetic valve,
which operates at repetition rate 1.25–5 Hz and is synchronized
with the laser pulses. The time delay between a laser pulse and
the valve opening is controlled using the timing module in or-
der to manage and optimize the process of cluster formation. In
our work, we used pure argon gas for cluster production. The
maximum value of the gas backing pressure that we used was
2 MPa though the working pressure in the vacuum chamber
did not exceed 5 mtorr. Thus, the mean radius of argon clusters
estimated according to the Hagena law modified for large clus-
ters [13] was 20 nm. Rayleigh scattering experiments showed
that the Hagena law gives the overestimated cluster size, and
in [25], the correction of the Hagena law was proposed. The
authors established experimentally that the average cluster size,
which is characterized by the number of atoms in a cluster Nexp ,
is related with Ntheor —The number of atoms in a cluster esti-
mated from the Hagena law as Nexp = Ntheor · η −2 , here η is the
dimension ratio obtained in [25]. In our experiments, the laser
beam was focused 5 mm below the nozzle outlet and the mean
cluster radius at the distance of 5 mm from the nozzle outlet was
estimated to be 14 nm.
According to [26], the cluster fraction in gas-cluster mixture
rises steadily when the valve opening duration varies from 300
to 800 μs. In our experiments, the valve opening duration was
400 μs. Estimates show that the cluster fraction for 400 μs
opening duration is 10%–12%, that corresponds to the cluster
density of about 5 · 1011 cm−3 .
The general scheme of our experiment in single-color and
dual-color excitation regimes is depicted in Figs. 1 and 2. The
laser beam is focused into the cluster jet by L1 lens (F = 20 cm)
at the distance of 5 mm below the nozzle outlet edge as has
been mentioned above. The exit window of the vacuum grating
72 IEEE TRANSACTIONS ON TERAHERTZ SCIENCE AND TECHNOLOGY, VOL. 7, NO. 1, JANUARY 2017
Fig. 1. Experimental setup of laser-cluster beam interaction: side view.
Fig. 2. Experimental setup of laser-cluster beam interaction: top view.
compressor and the entrance window of the vacuum chamber,
and focusing lens L1 are fabricated of MgF2 , which has low
value of n2 nonlinear refraction index. That allowed us to avoid
the influence of self-interaction effects in the laser beam on its
propagation path.
As shown in Figs. 1 and 2, the experimental setup provides
both single-color and dual-color regimes of the cluster jet exci-
tation. Beta Barium Borate (BBO) crystal (Type 1, thickness of
200 μm) placed inside the vacuum chamber close to the entrance
window is used to generate second harmonic collinearly to the
fundamental laser beam in the dual-color excitation scheme.
BBO crystal can be removed from the fundamental beam path
to provide the single-color regime of the cluster jet excitation.
The fundamental beam is linearly polarized in the horizontal
plane. The polarization plane of second harmonic in our exper-
iments was defined by the orientation of BBO crystal and was
kept at about 70◦ as related to the horizontal plane.
THz radiation generated in the gas beam is collected in two
directions: in the “forward direction” and in the “angular direc-
tion” at the angle of 30◦ in relation to the optical-axis in the
horizontal plane as shown in Fig. 2. L2 and L3 lenses fabricated
of polypropylene are used to collect THz radiation emitted in the
“forward direction.” THz signal emitted in the “angular direc-
tion” is collected by a pair of off-axis parabolic mirrors PM1 and
PM2. The optical axis of PM1 mirror is oriented at 30◦ to prop-
agation direction of the laser beam. As we already mentioned
in Section I, in [8]–[10] it was reported that the angular pattern
of THz radiation generated in the argon cluster beam demon-
strates four-lobed angular distribution. In our experiments, PM1
mirror collects THz radiation from one of the significant peaks
of power angular distribution, which is located at about 30◦ to
laser beam axis. THz radiation is leaving the vacuum chamber
through polypropylene windows with the transmission band of
0–3.5 THz, and is detected with standard 4.2 K silicon bolometer
system with preamplifier LN-6/C (Infrared Laboratories, Inc.).
X-ray yield from the nanoplasma is measured by a photo-
multiplier tube (PMT) equipped with NaI scintillator of 5 mm
thick and 25 mm diameter. PMT is placed behind beryllium
window of the vacuum chamber, which transmits X-ray radi-
ation with quanta energy above 2 keV. PMT is positioned at
the angle of 135◦ relative to laser beam propagation direction
as shown in Fig. 2. The X-ray spectrum was measured by Si-
PIN diode (model XR-100CR, Amptek, Inc.,) in a range of
2–30 keV with the energy resolution of about 200 eV. The
X-ray source size was measured with the use of X-ray matrix
detector Medipix2 CMOS ASIC based on CdTe crystal of 2 mm
thickness with 1128 pixels × 128 pixels format and pixel size of
110 μm × 100 μm. The side-scatter image of the plasma fila-
ment was controlled with the charge-coupled device camera.
III. EXPERIMENTAL RESULTS
A. Single-Color Excitation Regime
The energy spectrum of X-ray radiation generated from the
argon cluster beam under single-color excitation regime is de-
picted in Fig. 3. The presence of the gap in the energy spectrum
in the range of 3.5–5 keV is explained by the measurement pro-
cedure: the K-line (“left” part) and background (“right” part)
of the spectrum were measured separately and different sets
of filters and diaphragms were used in each case to achieve
the single-photon mode of the X-ray spectrometer. It has to
be noted that X-ray emission around K-line has its own back-
ground. However, it is not shown in Fig. 3.
There are two effective methods to study the process of cluster
formation in the supersonic jet: with the help of pyroelectric de-
tector placed into the jet [16] and using the analysis of properties
of X-ray radiation [1] by means of femtosecond photo-excitation
of gas cluster mixture. For our experimental conditions, the
generation of strong characteristic line in the X-ray spectrum
(E ≈ 3 keV, K-line of argon) on the one hand, confirms the oc-
currence of clusterization and the presence of argon clusters, and
on the other hand creates a source of powerful X-ray radiation.
In the gas medium, the K-line X-rays can be generated effi-
ciently if the ponderomotive potential of electrons in the laser
BALAKIN et al.: INTERACTION OF HIGH-INTENSITY FEMTOSECOND RADIATION WITH GAS CLUSTER BEAM
Fig. 3. Energy spectrum of X-rays generated under excitation of argon clusters
by femtosecond laser pulses focused on the front edge of cluster jet. Single-
color excitation regime, laser pulse energy 20 mJ, pulse duration 250 fs (negative
chirp), argon backing pressure 2 MPa.
field exceeds the ionization potential of argon K-shell. The
ponderomotive potential of electrons according to [1] could
be estimated as Up = 9.3 · 10−14 ·I [W/cm2 ]·λ2 [μm2 ]. In our
experimental conditions, the laser pulse intensity was about
3 · 1016 W/cm2 that corresponds to Up = 1.8 keV, whereas the
ionization potential of argon K-shell is 3.2 keV. The ionization of
the K-shell at the laser intensities of about 1016 − 1017 W/cm2
can take place only in plasma with solid density. In this case,
free electrons can absorb laser energy efficiently either via
bremsstrahlung effect, i.e., each time when scattered by the ions
or via resonant absorption mechanism [15]. That is why, only
the dense nanoplasma originating from ionization of clusters
can provide the generation of the detected X-ray line.
The contrast of K-line of argon, i.e., the ratio of line ampli-
tude to the amplitude of X-ray background is about 90 that is
higher than the contrast obtained in other experimental works
[27], [28]. The approximation of continuous X-ray background
by an exponential function allows us to estimate the energy (a
so-called “temperature”) of hot electrons as T1 = 1.4 keV. Due
to the high contrast of X-ray K-line, it was possible to detect
integral X-ray yield online at each laser pulse using the PMT
detector equipped with NaI scintillator. Therefore, all simulta-
neous measurements of THz and X-ray signals to be discussed
below were performed using the PMT detector for X-ray reg-
istration. The total energy of all X-ray quanta that reached the
scintillator was measured in each laser pulse. Taking into ac-
count a solid angle that corresponds to PMT position and X-ray
line generation efficiency, the estimated number of X-ray char-
acteristic photons that was registered in each laser pulse can
reach 105 . X-ray yield that corresponds to different positions
of PMT, i.e., 135◦ and 45◦ from laser beam propagation direc-
tion appeared to be the same. Therefore, we assume that X-ray
radiation is almost isotropic.
We have estimated the efficiency of generation of X-ray K-
line in argon clusters (E ≈ 3 keV) when argon backing pressure
was 2 MPa. The efficiency of K-line generation was 2 · 10−6
73
Fig. 4. THz and X-ray yield from argon cluster jet as a function of laser pulse
duration. Single-color excitation regime, laser pulse energy 22.7 mJ, argon
backing pressure 2 MPa.
when the negatively chirped laser pulse with duration τ ≈
250 fs and energy E ≈ 20 mJ was focused on the front edge of
the cluster jet. The efficiency raised up to 7 · 10−6 in the case
when transform-limited laser pulse (τ ≈ 50 fs, E ≈ 25 mJ) was
applied. The measured estimated X-ray generation efficiency
was the same order with an efficiency obtained in our previous
experiments that were carried out with argon clusters excited
by the laser pulse with the energy of about 5 mJ focused at a
distance of 2 mm from the nozzle outlet [16], [17]. We suppose
that in the present experiment, the same efficiency was obtained
due to the larger distance between the interaction zone and the
nozzle outlet, i.e., smaller cluster size was compensated by the
larger laser pulse energy.
We measured the lateral dimension of the X-ray source using
knife-edge technique. The edge of a copper foil 100 μm thick
was used as a knife. The transmission of the foil at the 1/e level is
about 30 keV. Therefore, all X-ray radiation from cluster plasma
was absorbed by the foil. We found that the X-ray source spreads
out along the direction of the laser pulse propagation. The lateral
dimension of the source appeared to be 2.3 mm ± 0.3 mm and it
is in good agreement with the size obtained from the images of
plasma optical emission. We used this value for the elaboration
of a scheme for collecting THz radiation propagating at angular
direction relative to the laser beam axis.
In our experiments, THz emission generated under the single-
color excitation was observed only at the angle of 30◦ relative to
the direction of laser beam propagation. No THz signal from the
argon cluster beam was registered in the forward direction. Fig. 4
shows dependencies of the energy of THz and X-ray pulses
jointly generated from the argon cluster beam as a function of
laser pulse duration for both positively and negatively chirped
laser pulses. It can be seen that the THz yield decreases strongly
in the region of minimal duration of the laser pulse, whereas the
X-ray yield demonstrates maximum value. The minimal laser
pulse duration (and the maximal X-ray yield) is characterized
by the vacuum intensity 1.3·1017 W/cm2 of the laser radiation.
74 IEEE TRANSACTIONS ON TERAHERTZ SCIENCE AND TECHNOLOGY, VOL. 7, NO. 1, JANUARY 2017
Fig. 5. THz yield from argon cluster jet as a function of laser pulse duration at
various pulse energies: 6.5, 11.3, 22.7 mJ. Single-color excitation regime, argon
backing pressure 2 MPa.
Such large intensity is sufficient for the occurrence of nonlinear
resonant cluster heating mechanism.
The effect of the pulse duration on the X-ray yield from ar-
gon clusters irradiated with intensive femtosecond laser pulses
was observed in [4] and explained by a nonlinear resonance ab-
sorption process, which involves energetic electron oscillations
back and forth through the cluster. As the laser pulse duration
increases the laser intensity reduces, the heating mechanism
changes to the linear one that results in X-ray yield decrease.
Similar behavior of X-ray yield for various pulse durations was
observed in our work and shown in Fig. 4.
Initially we assumed that the THz radiation could be absorbed
in the dense cluster plasma generated by the laser field of high
intensity, because laser intensity takes the maximum value at
minimal pulse duration for a given total energy of laser pulse.
To verify this idea, we measured the THz yield as a function
of optical pulse duration at three different levels of laser exci-
tation energy. It is clearly seen from Fig. 5 that all three curves
demonstrate the same behavior and their shape does not depend
on the total energy of the laser pulses at three given values of
the energy.
B. Dual-Color Excitation Regime
Under the dual-color excitation regime of the argon cluster
jet, we registered THz emission in both the forward and angu-
lar directions. The THz emission yield in the direction of 30◦
relative to direction of laser beam propagation was one order
of magnitude larger than in the forward direction. The ratio be-
tween absolute values of these two THz signals was estimated
taking into account the difference in the collection and prop-
agation conditions of the THz beams in forward and angular
directions. Besides, the use of the dual-color excitation regime
gives about fivefold increase in the THz yield compared with the
single-color excitation regime (when comparing the THz signals
generated under optimal conditions for both cases). The X-ray
Fig. 6. THz signal from argon cluster jet as a function of laser pulse duration
in two cases: emission at 30◦ relative to direction of laser beam propagation,
and in forward direction. Dual-color excitation regime, argon backing pressure
2 MPa.
emission yield did not demonstrate any changes after switch-
ing from the single-color to the dual-color regime. Moreover, in
our experiments, the X-ray yield did not depend on the angular
orientation of the BBO crystal.
The curves shown in Fig. 6 represent the dependencies of
energy of the THz pulses generated from the argon cluster jet
at the angle of 30◦ relative to the laser beam and in the for-
ward direction along the laser beam path; both dependencies
were measured as functions of the laser pulse duration. As one
can see from Fig. 6, the magnitude of THz signal collected at
the angle of 30◦ relative to the laser beam axis decreases in
the region of the minimal duration of the laser pulses, but the
depth of the dip is not as strong as in the case of single-color
excitation regime. In contrast, the THz signal collected in the
forward direction grows up to a maximal value when the ex-
citant laser pulse becomes the shortest. We assume that THz
emission in the forward direction originates from the interac-
tion of the dual-color laser pulses with nonclustered gas. The
condensation degree of argon in the cluster jet under our exper-
imental conditions was estimated as 10%–12%; therefore, the
percentage of monomers (noncauterized atoms) in the argon jet
was about 90%. Therefore, THz emission in the forward direc-
tion could originate from the four-wave mixing (FWM) process
(2ω − ω − ω) and transient photocurrent J(t) similar to the case
of THz generation under optical breakdown in gas-phase me-
dia with dual-color laser pulses. In this case, the THz yield is
maximal when the laser intensity reaches maximum value (at
the shortest duration of the laser pulse) because the efficiency of
FWM process and photoionization rate both are maximal under
these conditions.
In addition, it can be seen in Figs. 4–6 that positively chirped
excitant pulse results in a higher THz yield as compared with
the negatively chirped one. We suggest that this effect can be
explained by a spectral asymmetry of the laser pulses provided
by our laser system. As shown in [29], because of the spectral
asymmetry a chirped pulse in the time domain has the “shoulder”
BALAKIN et al.: INTERACTION OF HIGH-INTENSITY FEMTOSECOND RADIATION WITH GAS CLUSTER BEAM
located on either the leading or trailing edge of the main pulse
depending on the sign of the chirp. If the “shoulder” is located
on the leading edge of the pulse, it acts as a prepulse and affects
the laser–cluster interaction.
The measurements of THz pulse energy were carried out
with fixed laser excitation energy in two schemes of laser action
on the cluster beam: with single-color action at ω frequency
and at dual-color action at ω + 2ω. In both schemes, the total
energy of laser radiation remained unchanged and its conversion
into the second harmonic in BBO crystal did not exceed 10%.
In our experiments, we used the laser system with low-pulse
repetition rate and relatively high-energy fluctuations, which
did not allow us to measure the field strength according the
techniques described, for example, in [30] and we measured the
THz pulse energy. We used Golay cell detector (model GC-1P,
Tydex) which was calibrated by us for the measurement of THz
pulse energy and received the following results. Every time the
measurements were carried out for the maximal energy of THz
pulse; and for its optimization, the duration of laser pulse was
changed in accordance with the measurement results shown in
Figs. 4 and 5. When measuring at the angle of 30◦ with excitant
laser pulse energy of 9 mJ, the energy of THz pulse was about
0.6 nJ in single-color and 3 nJ in dual-color laser excitation
regime, respectively. Here, we have to note that with in our
experimental setup (see Section II), we did not collect all THz
radiation because it has complex conical spatial distribution,
which is described, for example, in [10]. In our experiments,
the THz radiation is collected in a solid angle of 0.2 sr which
is provided by PM1 parabolic mirror (see Fig. 2). We evaluated
the energy of THz pulse in forward direction only in the case of
double-color interaction and it was 0.15 nJ. In the single-color
regime, no signal was observed in the forward direction.
IV. MODEL OF IONIZATION AND EVOLUTION OF THE
ARGON CLUSTER
We assume that the abovedescribed dependency of the X-ray
and THz yields upon the laser pulse duration can be attributed to
some peculiarities of the free electron production in cluster and
cluster evolution itself [31]. In particular, one needs to explain
why a maximum of X-ray yield is achieved at the minimal
duration 50 fs of the laser pulse in contrast to the decline of the
THz yield at the minimal duration of excitant pulse, while the
THz yield grows up to a maximal value when the pulse duration
increases up to 250 fs. Here, we do not give strict theoretical
interpretation of this phenomenon, but the following remarks
show that it is connected with the dynamic process of cluster
ionization by a pulse of a femtosecond laser [32]. The maximal
intensity of laser radiation in our experiments was Imax = 1.3 ·
1017 W/cm2 , and it corresponded to the shortest laser pulse of
about 50 fs. The intensity of laser field in the focus of such pulse
typically exceeds the intensity of an intrafield, which could be
estimated for a hydrogen atom at the first Bohr orbit with radius
aB ≈0.05 nm according to a well-known formula as
e ing laser field on the cluster gradually leads to the forma-
E0 = ≈ 5 · 109 [V/cm] (1)
a2B
75
where e is the elementary charge. Consequently, the character-
istic energy flux density is
cE02
I0 = ≈ 3.5 · 1016 [W/cm2 ]. (2)
8π
With these parameters, the barrier-suppression ionization be-
comes possible, which means that an atomic electron is just
pulled out from the atom by the laser field. According to the
existing theoretical description of the barrier-suppression ion-
ization [18], [19], [31], the collapse of an atom its transformation
into an ion with charge state Z occurs when the external electric
field strength exceeds the critical value
JZ2
Ecr = (3)
4e4 Z
where Z is the ion charge state and Jz is ionization potential to
the specified state. The ionization produces free electrons with
equal probability both in cluster and in gas.
According to [33], ionization potentials for the first 11 elec-
trons in argon atom are 15.756, 27.62, 40.90, 59.79, 75.0, 91.3,
123.9, 143.4, 422.6, 479.0, and 539.5 eV, respectively. Thereby,
Jz increases almost three times between 8th and 9th electrons
when Jz jumps from J8 = 143.4 eV to J9 = 422.6 eV. The
required laser field strength increases 7.7 times from 0.87E0 to
6.7E0 , accordingly, which corresponds to the increase of pulse
intensity about 60 times from I8 = 2.64·1016 W/cm2 to I9 =
1.58·1018 W/cm2 . Since the intensity of the laser field did not ex-
ceed Imax = 1.3·1017 W/cm2 in our experiments, the ion charge
state Z was fixed at the level of 7–8. The chirping of the laser
pulse could not change this value because Imax changes only by
a factor of 12 in the range of the pulse duration variation. For
the first eight levels of argon, the ionization potential is almost
proportional to Z and can be evaluated as JZ ≈ 16.5Z eV. Ac-
cording to [31], the time of ionization of these levels could be
estimated as
√ 2 √
2e Z me
τZ ∼ 3/2
∼ 10−16 Z −1 [s] (4)
Jz
where me is the mass of electron. Therefore, one may consider
that the ionization occurs almost immediately, for the time less
than a oscillation period of the laser field.
The deeper levels with Z ≥ 9 could be ionized due to the
mechanism of impact ionization. Indeed, we note that any free
electron in the laser field with electric field strength E at fre-
quency ω gains the energy of the order of
 2
me eE I
W = = 4300 [eV ] (5)
2 me ω I0
which exceeds the energy of ionization of deeper levels. How-
ever, the process of impact electron ionization takes few tens of
femtoseconds inside clusters and much longer time in the gas.
We assume that the interaction of a femtosecond laser pulse
with argon cluster leads to the formation a quasi-neutral plasma
inside the cluster core. The quasi-neutrality persists during the
initial stage of laser pulse propagation. The action of the ris-
tion of nonuniform radial distribution of ions, which is almost
76 IEEE TRANSACTIONS ON TERAHERTZ SCIENCE AND TECHNOLOGY, VOL. 7, NO. 1, JANUARY 2017
spherically symmetric; and the formation of asymmetric distri-
bution of the electrons, which oscillate between the poles of the
cluster [34]. The laser field pulls the big chunks of electrons out
of the cluster every half period of the field oscillations, while
the ion cloud gradually expands in the radial direction. Because
of the fast losses of electrons, the cluster gradually acquires a
net electric charge Q. This pattern is due to the different field
strength in different parts of the cluster. Indeed, the total electric
field acting on the single ion is composed of an external laser
field averaged over a period of the laser field, own static field
of the charged cluster and the dynamic field associated with the
forced oscillations of the electron cloud in the cluster. On the
contrary, the electrons are quick enough to follow the phase of
the laser field.
To evaluate Q, we suppose that the charge density is evenly
distributed across the cluster, so that the static field is radially
symmetric and given by
Qr
EQ (r) = (6)
R2
where r and R are the distances to the center of the cluster and
the cluster radius, respectively. Using the relation between the
cluster charge and laser field strength as Q(R) = 4ER2 , one
can obtain
EQ (R) = 4E. (7)
This field has a radial distribution which leads to the fact that
under the action of the laser pulse the total field of the cluster
charge at the poles and at the equator of the cluster will be
different. Indeed, the fields applied to the poles are collinear
and their sum
√ is equal to 5E, whereas the sum value at the
equator is 17E, since these fields are orthogonal. We suggest
that the difference between the field amplitude at the poles and
the equator could be much larger due to the nonuniformity of
the spatial distribution of electrons. As reported in [35], the
polarization-induced electric field at the poles exceeds the laser
electric field by up to an order of magnitude. This might be
sufficient for ionizing the ninth and subsequent electrons from
argon ion, but further calculations are needed to verify this
assumption. In any case, the number of free electrons produced
as a result of barrier-suppression ionization seems to be so large
that the corresponding plasma frequency is at least an order of
magnitude higher than we could detect in our measurements.
We conclude, therefore, that the observed THz radiation is not
produced by the plasma oscillations of electron cloud in the
vicinity of a single cluster.
V. ANGULAR PATTERN OF THZ RADIATION
Following [10], we assume that the THz radiation produced
by the first harmonic of the laser radiation is generated by a time-
varying axially symmetric linear quadrupole, which is produced
by the ponderomotive force of the laser pulse. Under the action
of the ponderomotive force, the plasma filament produced by
the laser pulse first expands radially and then shrinks back after
the propagation of the laser pulse thus forming the time-varying
linear quadrupole. As shown in [8], the waveform of THz ra-
diated pulse comprises two half-periods corresponding to the
onefold radial expansion and subsequent compression of the
filament. Jahangiri et al. [10] developed a phenomenological
model of the THz radiation that takes into account the effect of
finite length L of the filament, which is larger than the wave-
length λ of the THz radiation. They showed that the transition
radiation [36] and transition-Cherenkov radiation [37] could not
explain angular distribution of THz radiation pattern from the
clustered plasma, which was observed in a number of experi-
ments. Quadrupole low-frequency emission of plasma channel,
created by femtosecond laser pulse in gaseous medium, was
studied theoretically in [38]. The interference of quadrupole
THz sources in the plasma channel results in the formation of
angular distribution of THz field, which has a minimal value
on the filament axis and achieves maximum value at the angle
Θmax between detector and filament axis. The value of Θmax is
given by the following formula:

Θmax = 69◦ λ/L. (8)
As has already been mentioned in Section III-A, the filament
length in our experiments was 2.3 mm and hence the angle of
THz emission at frequency f = 0.7 THz may be estimated as
θ = 30◦ . It is also worth noting that in [9] the length of the
plasma channel created in the cluster jet was varied by the F-
number of focusing lens. It was found that angle of maximum
of √the THz emission is proportional to the plasma length L as
1/ L which is in agreement  with (8).
An estimation Θmax = 2λ/L similar to (8) was derived in
[39] for a dipole radiation of the plasma filament, which be-
comes significant in the two-color scheme. As shown in [39],
angular distribution of the dipole radiation is very sensitive to
the polarization of the second harmonic regarding the first har-
monic. In the case where the polarization of second harmonic
is perpendicular to the first one, as it was in our experiment, the
dipole THz radiation has maximum in the forward direction,
and Θmax = 0 . Our experiments confirm this conclusion, as we
observed THz radiation in the forward direction only in case of
two-color scheme.
VI. CONCLUSION
We have found that the yield of THz and X-ray radiation from
the argon cluster beam, excited by high-intensity femtosecond
laser pulses, depends differently on the laser pulse duration.
THz yield strongly decreases when laser pulse duration is the
shortest, whereas X-ray yield is maximal under these conditions.
The formation of spatial distribution under 30◦ is connected
with the dynamics of radial oscillations and, therefore, has such
complex dependence on the pulse duration. X-ray emission does
not depend on such dynamics and grows proportionally to the
growth of the laser intensity.
The difference in the optimal laser pulse duration for the effi-
cient generation of X-ray and THz radiation can be explained by
the different time periods required for the formation of electron
subsystems in argon cluster. The population of outer electrons
rises quickly during the first 50 fs and they are responsible for
the generation of X-ray, which explains the maximal X-ray yield
at the minimal pulse duration in our experiments. The inner
BALAKIN et al.: INTERACTION OF HIGH-INTENSITY FEMTOSECOND RADIATION WITH GAS CLUSTER BEAM
electrons multiply slowly and their population reaches maxi-
mum at the time scale of about hundreds femtoseconds, which
can be attributed to the enhancement of THz yield at τ ≈ 250 fs
in our experiments. At the later stages, the population of outer
electrons begins to rise again that may cause the decrease in the
THz signal.
The use of dual-color excitation scheme results in ∼5-fold
enhancement of the THz yield while the yield of the X-ray
radiation remains the same and energy conversion efficiency to
the K-line is about 7·10−6 .
ACKNOWLEDGMENT
The authors would like to thank Prof. X.-C. Zhang for fruitful
cooperation at all stages of work on this paper, I. V. Timofeev for
useful discussion on clusters dynamics, and A. Y. Sidorov for
the assistance in the experiments. The authors would also thank
A. A. Shkurinova for reading and correcting the English version
of this paper’s manuscript.
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Alexei V. Balakin received the M.S. degree in
physics and Ph.D. degree in physical and mathemati-
cal science (with a specialty in laser physics) from M.
V. Lomonosov Moscow State University, Moscow,
Russia, in 1995 and 1998, respectively.
Since 1998, he has been a member of the Physics
Faculty of M. V. Lomonosov Moscow State Univer-
sity. He is currently a Researcher. He has authored
more than 65 articles and theses. His research in-
terests include laser physics and nonlinear optics
and nonlinear interaction of femtosecond laser pulses
with optically isotropic-active media, generation, and application of high-power
terahertz pulses in terahertz spectroscopy.
Murat S. Dzhidzhoev was born in Tzkhinval, South
Ossetia, in 1938. He received the graduate and
Ph.D. degrees from the Faculty of Physics, M.
V. Lomonosov Moscow State University (MSU),
Moscow, Russia, in 1963 and in 1972, respectively.
He specializes in laser physics and profound stud-
ies of X-ray and terahertz radiation of femtosec-
ond cluster nanoplasma. He received the Lomonosov
Conference Diploma. He has conducted research on
nonlinear excitation of pure ozone molecules. He is
currently a Senior Scientific Researcher with the De-
partment of General Physics and Wave Processes, Faculty of Physics, M. V.
Lomonosov MSU.
Vyacheslav M. Gordienko received the graduate,
Ph.D., and Dr. Sci. degrees in physics from M.
V. Lomonosov Moscow State University, Moscow,
Russia.
He is the Head of the R. V. Khokhlov Nonlinear
Optics Laboratory. He has made a significant contri-
bution to the development and creation of powerful
pico and femtosecond laser systems operating in UV,
visible, and mid-infrared spectral ranges. He has car-
ried out a number of fundamental studies aimed at
studying the nonlinear interactions of intense ultra-
short laser radiation with matter in strongly nonequilibrium condition. The
results of his scientific research have been published in leading scientific jour-
nals. He has authored about 200 scientific papers.
Mikhail N. Esaulkov received the M.Sc. degree in
physics from the Moscow Institute of Physics and
Technology, Moscow, Russia, in 2010.
Since 2007, he has been a Member of the group led
by Prof. Alexander Shkurinov with the Department
of Physics, M. V. Lomonosov Moscow State Uni-
versity, and since 2014, with the Institute for Laser
and Information Technologies, Russian Academy of
Sciences. He has authored or co-authored 11 papers
in peer-reviewed scientific journals and 14 papers in
conference proceedings. His research area and Ph.D.
thesis are related to the processes of generation and detection of THz radiation
in the gaseous media and plasma of optical breakdown. His research interests
include nonlinear optics, surface physics, generation of THz radiation in gases
and thin films, and polarization of the THz radiation.
Irina A. Zhvaniya received the degrees in physics
and Ph.D. degree from M. V. Lomonosov Moscow
State University (MSU), Moscow, Russia, in 2008
and 2014, respectively. Her Ph.D research concerned
X-ray and harmonics generation under interaction of
femtosecond laser with solids and clusters.
She is currently working with MSU as a
Researcher.
Konstantin A. Ivanov received the graduate degree
from M. V. Lomonosov Moscow State University,
Moscow, Russia, in 2010.
He is a Researcher with the Physics Faculty of
Moscow State University. His scientific interests in-
clude interaction of high-power femtosecond laser ra-
diation with matter (solids, structured target, liquids,
etc.) and investigation of hot electron acceleration
and hard X-ray generation.
Igor A. Kotelnikov received the graduate degree
from Novosibirsk State University, Novosibirsk,
Russia, in 1981.
He is currently a Chief Scientist with the Bud-
ker Institute of Nuclear Physics, Novosibirsk, and a
Professor in the Plasma Physics Chair, Novosibirsk
State University. His research interests include con-
finement, equilibrium, and stability of quasi-neutral
and nonneutral plasmas.
Nikolay A. Kuzechkin received the M.Sc. degree in
physics from M. V. Lomonosov Moscow State Uni-
versity, Moscow, Russia, in 2015.
He is currently with the Laboratory of Tera-
hertz Photonics and Information Technologies, Insti-
tute on Laser and Information Technologies, Russian
Academy of Sciences, Moscow. His research inter-
ests include terahertz generation in laser-produced
plasma, interaction of intense ultrashort laser pulses
with atomic and molecular clusters, and terahertz
spectroscopy.
BALAKIN et al.: INTERACTION OF HIGH-INTENSITY FEMTOSECOND RADIATION WITH GAS CLUSTER BEAM
Ilya A. Ozheredov received the graduate and Ph.D.
degrees from M. V. Lomonosov Moscow State
University, Moscow, Russia, in 1995 and 2001,
respectively.
He is an Associate Professor with the Chair of
General Physics and Wave Processes, Department of
Physics, M. V. Lomonosov Moscow State University.
His research interests include nonlinear optical spec-
troscopy, laser physics, vacuum physics, and surface
science. His current research interests include scien-
tific activity on THz optoelectronics and photonics.
Vladislav Y. Panchenko received the graduate de-
gree from the Faculty of Physics, M. V. Lomonosov
Moscow State University (MSU), Moscow, Russia,
in 1971.
In 1994, he became a Professor with MSU. Since
2008, he has been a Full Member of the Russian
Academy of Sciences. He is the Director of the In-
stitute of Molecular Physics, Russian Science Center
“Kourchatovsky Institute” and the Board Chairman
of the Russian Foundation for Basic Research. From
1998 to 2006, he was the President of the Russian
Chapter of International Society for Optical Engineering and a Member of the
International Directorate of OSA. He has authored or co-authored 14 mono-
graphs and more than 400 collected papers and articles in the field of nonlinear
kinetics in molecular systems, laser-matter interaction, laser material process-
ing and laser micronanotechnology, lasers and information technologies for
biomedical applications, and medical physics.
Prof. Panchenko is the Knight of the Legion of Honour (France) and Cavalier
of the UNESCO Medal for contributions to the development of nanoscience and
nanotechnologies.
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Andrey B. Savel’ev received the Ph.D. and Dr. Sc.
degrees from M. V. Lomonosov Moscow State Uni-
versity (MSU), Moscow, Russia, in 1989 and 2004,
respectively.
He is currently a Professor with MSU. He has
authored or co-authored more than 100 scientific pa-
pers. His research interests include interaction of su-
perintense light fields with matter, charged particle
acceleration in laser plasma, and femtosecond non-
linear optics.
Mikhail B. Smirnov, photograph and biography not available at the time of
publication.
Peter M. Solyankin, photograph and biography not available at the time of
publication.
Alexander P. Shkurinov received the graduate and
Ph.D. degrees in physics from M. V. Lomonosov
Moscow State University (MSU), Moscow, Russia,
in 1985 and 1988, respectively.
Since 2015, he has been a Professor with the De-
partment of Physics, M. V. Lomonosov MSU. His re-
search interests include the development and applica-
tion of femtosecond laser techniques, time-resolved
spectroscopy of molecules in liquid phase, nonlinear
optics, and THz techniques and spectroscopy. The re-
sults obtained by him have been published in more
than 100 scientific papers in peerreviewed journals.
Dr. Shkurinov was the recipient of the Medal in Honor of Prof. Rozhdestven-
sky for his contribution into the development of optical science and technology
from The Russian Optical Society.