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 Astro Ltd Laser Physics

Laser Phys. 30 (2020) 036002 (13pp) https://doi.org/10.1088/1555-6611/ab67cc

Scaling up and parametric characterization

of two-color air plasma terahertz source
S Saxena1,2, S Bagchi2, M Tayyab1,2, B S Rao1,2, S Kumar3, D N Gupta3 and
J A Chakera1,2
1
  Homi Bhabha National Institute, Training School Complex, Anushakti Nagar, Mumbai 400 094, India
2
  Laser Plasma Division, Raja Ramanna Centre for Advanced Technology, Indore 452 013, India
3
  Department of Physics and Astrophysics, University of Delhi, Delhi 110007, India

E-mail: sbagchi@rrcat.gov.in

Received 3 July 2019

Accepted for publication 28 December 2019
Published 3 February 2020

Abstract
The plasma produced by frequency mixing of an ultrafast pulsed laser and its second-
harmonic field in air is a promising, table-top source of terahertz radiation. To maximize the
generation efficiency of such a source, multi-parameter optimization is essential. A parametric
study involving various external controls is presented here. Starting from the optimization
of phase and polarization of the second-harmonic field, the effect of laser intensity on the
terahertz flux is reported. Moreover, the effect of external focusing conditions, such as focal
length of the lens and effect of laser beam aperture, is explored in detail. Contrary to the
previous reports, we find that with the increase of laser intensity, terahertz (THz) flux increases
with more conversion efficiency; this is attributed to the multiple ionization of the air, leading
to stacked release of contributory electrons. Exploration of beam convergence reveals that
relatively weaker focusing leads to increased terahertz production compared to sharp focusing
conditions. Moreover, temporal characterization of the emitted terahertz pulse conducted
using electro-optic sampling provides pulse duration of 368 fs with corresponding frequency
spectra up to 3.6 THz. The maximum electric field of the terahertz pulse is estimated to be
1.12 MV cm−1 in our experimental conditions. Results of 2D particle-in-cell simulations are
also presented with the objective of validating the role of transient photocurrent mechanism
in THz generation from two-color laser-induced gas plasma. We believe the broadband, bright
THz source presented here will be useful in the imaging of bigger samples as well as nonlinear
spectroscopy.

Keywords: terahertz (THz) generation, ultrashort laser pulses, air plasma, electro-optic
detection, PIC simulation

Introduction known, and copious explorations have been performed in

In recent times, there has been a surge of scientific explora-
tion in the not-so-well-chartered territory of terahertz (THz)
radiation owing to its unique characteristics. Conventionally,
the radiation lying within the range of 0.1–10 THz is termed
as THz radiation. Though the primary motivation behind this
exploration was to investigate the internal structures of sol-
ids and large biomolecules, at present, its applications have
spread across diverse faculties of science and technology. It
is interesting to note that the THz range falls in between the
far-infrared and microwave regions, both of which are well
these regions. However, the lack of efficient generation and
proper detection mechanisms have hindered development in
the THz regime. In the last two decades, these problems have
been addressed and, based on the findings, a plethora of sci-
entific explorations are being performed [1, 2]. THz radiation
properties are exploited by a wide variety of groups related
to astronomy [3, 4], communication [5], defense and secu-
rity [6], disease detection [7], non-destructive testing [8],
pharmaceuticals [9, 10], and many other disciplines [11–14].
All of these applications rely on either of the two major tech-
niques, namely THz imaging [15, 16] and THz time-domain

1555-6611/ 20 /036002+13$33.00 1 © 2020 Astro Ltd  Printed in the UK

Laser Phys. 30 (2020) 036002
techniques [17–19], and are very much dependent on the
development of a bright, broadband, tabletop source of THz
[20]. The approach towards the THz frequency range can be
primarily divided in to two branches: (i) the frequency down-
conversion, i.e. the photonic approach [21], and (ii) frequency
up-conversion, i.e. the electronic approach [22, 23]. Both
these approaches are at present vividly being pursued keeping
prospective applications in mind. The present study follows
the photonics route to producing THz radiation.
The photonics approach is largely based on ultrashort-
duration pulsed lasers. Apart from the solid-state sources such
as photoconductive antennas [24] and non-linear crystals [25],
lasers have proven to be effective in generating THz radia-
tion from the fourth state of matter, i.e., plasma. Plasma, as
an already disintegrated medium, stands out among all the
alternatives available, leaving no concerns related to mat­
erial damage [26, 27]. THz generation from ionized gas was
first reported by Hamster et  al in 1993 [28]. Laser with 50
mJ energy was focused on a He gas target, and less than 10−6
conversion efficiency was obtained. In the year 2000, Loffler
et  al demonstrated THz generation from ambient air, which
included application of DC bias across the plasma filament
[29]. Detectable THz could now be attained at as low as 1 mJ
laser energy. However, this technique was largely limited by
the rapid saturation with laser energy and electrical bias. THz
production through the application of AC bias on air plasma
by means of second harmonic of the laser was reported later in
the same year by Cook and Hochstrasser [30]. THz generation
by two-color laser-induced plasma in ambient air constituted
significant progress in the direction of achieving efficient THz
sources [31].
In this generation mechanism, an ultrashort laser pulse and
its second harmonic are co-focused in air to create a plasma
channel that emits an intense, single-cycle THz pulse in the
conically forward direction. Such an air-plasma-based THz
source provides broadband radiation [32–34] and a very high
THz field intensity [35, 36], features typical conversion effi-
ciency of 10−4 order [37] and has no vacuum requirements,
and the source is available in plenty. This bright, broadband
source has been found to be particularly useful for spectr­
oscopy applications such as THz-time domain spectroscopy
[38]. Focusing such strong THz radiation creates electric
fields more than hundreds of kV/cm [39]. These THz pulses
are used to access physical phenomena that are nonlinearly
dependent on the electric field, like excitation of Rydberg
states in atomic physics [40] and transient photoconductiv-
ity in optically excited semiconductors [41]. The ambient air
source of THz from two-color induced plasma is also an ideal
choice for remote THz generation and detection [33, 42, 43],
thereby avoiding propagation losses.
In this article, a detailed experimental investigation of
the parametric dependence of THz radiation from a ‘two-
color’ scheme is demonstrated. Theoretical analysis of the
observations has been made on the basis of an established
transient current proposition, also known as the photocur­
rent (PC) model [44]. Impact of the phase and polarization
of the second-harmonic electric field in THz generation is
2
S Saxena et al
reported and discussed. The influence of physically adjust-
ing the position and azimuthal angle of the second-harmonic
generation (SHG) crystal is supported by the analytical PC
model. Scaling of THz flux with laser energy, overcoming
the saturation effect [45], is reported. Analytical simulations
performed for our experimental parameters indicate the role
of multiple ioniz­ation of the plasma medium in increase of
laser to THz conversion efficiency at higher laser energies.
Strong THz radiation of 11.2 µJ for 40 mJ pump laser energy
is obtained. Increase in focal length of the laser converging
lens is shown to further the THz generation for the same laser
energy and produce a more directional THz beam. The effect
of focusing geometry is also studied by altering the laser
beam size. Apertured laser-supported larger plasma volume
and enhanced 19 µJ THz energy is obtained. Focused THz
spot size estimation was done by the knife-edge technique and
revealed 1.94 mm full width at half maximum (FWHM) diam-
eter. Electro-optic sampling (EOS) with ZnTe 〈1 1 0〉 crystal
is performed for temporal and spectral characterization of the
THz radiation. THz pulse duration was measured to be 368
fs FWHM. For these observed values of spot size and pulse
duration, the THz electric field amounts to 1.12 MV cm−1.
The present paper is structured as follows: section  (1)
describes the predictions of the basic photocurrent (PC)
mechanism, followed by (2) two-dimensional particle-in-cell
(2D-PIC) simulations to explore how the inclusion of laser
pulse propagation effect influences THz generation. We show
that the results of the PIC simulation support the contribution
of transient photocurrent to the THz generation mechanism.
Section  (3) reports the experimental results, describing the
dependence of the THz flux on (a) second-harmonic crystal
and (b) laser pulse energy. Further, the role of external focus-
ing conditions, namely the effect of (c) apertured laser beam
on THz generation and (d) focal length of the lens, is also
reported. The role of focal length of the lens on (e) THz beam
divergence is presented, followed by (f) determination of the
THz focal spot size and (g) frequency-domain characteriza-
tion of THz radiation using EOS measurement.
1.  The photocurrent model
Combining second harmonic of the laser with the ionizing
field enhances conversion efficiency by almost two orders of
magnitude [43]. THz radiation generation from the two-color
laser-induced ambient air plasma source was earlier attrib-
uted to the four-wave mixing nonlinear effect [30, 46, 47].
However, it was realized that the third-order non-linearity
χ(3) value of the air/gas medium is too low to explain the
ampl­itude of THz flux generated through this method. This
phenom­enon is best described by the Photocurrent Model
[31, 44, 48], and is briefly discussed in the following section.
A few experimental investigations [49] have also confirmed
the role of transient photocurrent in the THz generation from
the ‘two-color’ scheme.
At moderate laser intensities (~1014–15 W cm−2) that
are used in the experiment, the gas medium undergoes tun-
neling ionization, instantaneously generating a free electron
Laser Phys. 30 (2020) 036002
Figure 1.  Photocurrent model. (a) and (c) Combined electric field of fundamental (ω) and second-harmonic (2ω) frequencies with relative
phase difference of 0° and 90°. (b) and (d) Resultant transverse electron current corresponding to (a) and (c). The asymmetric non-zero
behavior of transverse current in the case of 90° phase difference between ω and 2ω can be distinctly observed. (e) Resultant THz spectra
with phase difference (θ) of 0° and 90°.
population. We use the Ammosov–Delone–Krainov (ADK)
tunneling ionization rate [50] to compute the time-varying
electron density, with multiple degrees of ionization taken
into account. The free electrons drift away from their parent
ions at velocity defined at the moment of ionization, and at
the same time oscillate along the laser polarization direction.
Addition of second-harmonic laser field to the fundamental
produces an asymmetric electric field expressed as EL(t)  =  Eω
cos ωt  +  E2ω cos (2ωt  +  θ). Eω and E2ω are the amplitude of
the fundamental and second-harmonic laser, respectively,
and θ is the relative phase difference between the two fields.
As can be seen in figures 1(a) and (c), when ω and 2ω are in
phase (i.e. θ  =  0), the combined electric field is nearly sym-
metric while, for a phase difference of π/2, the combined
electric field is asymmetric. Once the electrons are liberated
through ionization, the drift velocity of electrons is computed
as vd(t)  =  e [Eω sin ωt/(meω)  +  E2ω sin (2ωt  +  θ)]/(2meω).
With θ  =  π/2, a nonvanishing current is generated that adds
up during the driving laser pulse duration. The generated THz
field is proportional to the time gradient of transverse current
density J⊥  =  eNevd, where e and Ne are the electronic charge
and charge density, respectively. Figures 1(b) and (d) show the
normalized current density for relative phase differences of 0
and π/2. The resultant THz spectra, as shown in figure 1(e),
clearly exhibit the effect of relative phase difference on THz
generation. Collisional processes and the recombinations are
ignored in this model, as they occur on a picosecond timescale
which is much longer than the pump pulse duration.
Although the PC model has been very successful [44, 49]
in predicting the origin of THz radiation from ambient air and
gases, one major flaw of the model is that it does not take into
account the intricate dynamics of the laser pulse propagation
in the medium and phenomena associated with it. In order to
address this issue, we have used PIC simulation to validate the
photocurrent model.
3
S Saxena et al
2.  Validation of photocurrent model using
particle-in-cell simulation
We have done 2D-PIC simulation using EPOCH code [51]
to study the THz generation by single- as well as two-color
laser pulses. We have considered a simulation box of size 200
µm  ×  200 µm filled with nitrogen gas having atmospheric
density. The simulations are performed for a time period of
1000 fs, with data recorded at an interval of 1 fs. The laser
enters the simulation box from the left edge and propagates
along the  +x-direction with polarization along the z-direction.
For single-color laser, the wavelength of the laser pulse is
800 nm (ω), and for two-color laser pulses, the second har-
monic of the fundamental laser pulse (2ω) is included. The
two laser pulses have a Gaussian profile both in spatial and
temporal domains with beam waist of size, r0  =  10 µm and
pulse duration T0 of 50 fs. The peak intensity of the funda-
mental laser pulse is chosen to be 5  ×  1015 W cm−2, which
is sufficiently large to cause ionization of the nitrogen gas by
different mechanisms such as multi-photon, tunneling, and
above-threshold ionization. These mechanisms are incorpo-
rated into the simulation code.
In the earlier reported simulation results [52] for a single-
color laser pulse, the ponderomotive force associated with the
laser pulse causes the electron to oscillate in transverse as well
as in longitudinal direction. The transient currents associated
with these plasma oscillations were found to be responsible
for the observed feeble THz field. The polarization of the
electric field associated with this radiation is along the cur­
rent direction. The Ez and Ey  fields are therefore the same for
the single-color laser pulse. Spatial distribution of Ez for the
single-color pulse is shown in figure 2(a) at 600 fs after the
start of simulation. To get a better visualization of the radiated
field, the high-intensity laser field is filtered out by setting a
cut-off of  ±1 GV m−1 on the electric field magnitude. The
Laser Phys. 30 (2020) 036002 S Saxena et al

Figure 2.  Electric field (Ez) associated with THz radiation generated by (a) single-color laser at 600 fs and (b) two-color laser pulse with
a phase difference of π/2 at time t  =  300, 400, 500, and 600 fs; ‘t’ is the time elapsed since the origin of laser from the left side of the
simulation box. The resultant current density produced by the single- and two-color laser pulses during propagation is shown in (c) and (d).
(e) Line profiles of the electric field Ez measured at the point (+50 µm, −50 µm) with respect to the central origin of the simulation box
for single- and two-color laser pulses. (f) THz spectra of the line profiles depicted in (e) derived by Fourier transform. An evidently clear
signature of broadband THz radiation is observed for two-color laser pulses, while the single-color pulse shows no such radiation.

simulations are performed with two-color laser pulses as well.
The second-harmonic laser pulse is propagated simultane-
ously with the fundamental laser pulse with a phase difference
of ‘π/2’. We assign 20% of laser intensity to the second-har-
monic field. For the same laser intensity, the effect of pon-
deromotive force should not change. The spatial profile of the
radiated electric field for this intensity distribution between ω
and 2ω should remain the same, as the ponderomotive force
does not change with the introduction of the second-harmonic
laser. Ey  for this case is indeed the same. The electric field in
z-direction for this case is shown as snapshots at successive
instances in time (300, 400, 500, and 600 fs) in figure 2(b).
The entry of the laser pulse from the left side of the simulation
box is considered as the beginning of time, i.e. ‘t  =  0’. The
intense dark part represents the laser field, and wings repre-
sent the radiated terahertz field emitted in the conical direc-
tion. It can be seen from figure 2(b) that the electric field along
the z-direction is much higher for the two-color laser case than
for the single-color laser condition. With use of the two-color
laser, experimental results showing a high-intensity THz radi-
ation have also been reported [53]. THz polarization is shown
to be the same as that of the laser pulse. This THz radiation

4
Laser Phys. 30 (2020) 036002 S Saxena et al

generation can be explained with the help of the photocurrent

mechanism.
The following simulation results explain the role played
by the two-color laser pulse in the generation of intense THz
radiation, and show the significance of photocurrent effect
with pulsed laser propagation in gas. When the fundamental
laser propagates at 90° phase difference with its second har-
monic, the combined laser electric field becomes asymmetric
along the propagation direction (figure 1(c)). As a result, the
transverse photocurrent Jz attains an asymmetric profile under
the action of the laser field. In the case of the single-color
laser, the laser pulse remains symmetric and hence the cur­
rent remains symmetric along the propagation direction. To
demonstrate this feature, current density along the central axis
of the simulation box at a fixed point in time for the two cases Figure 3.  Experimental setup of the THz generation from two-
is shown in figure 2. Figures 2(c) and (d) are for ω alone and color laser-induced air plasma and detection using pyroelectric
calorimeter. Arrangement for transverse imaging of the plasma
ω with 2ω at ‘π/2’ phase difference, respectively. Due to the fluorescence is also shown.
asymmetric nature of the current density under the two-color
situation, there is a net transient current which is responsible
two-color laser pulses greatly improves the yield of THz radi-
for the intense electromagnetic radiation. Corresponding to
ation as compared to the use of single-color laser pulses [52].
the laser pulse duration in tens of femtoseconds, the radiated
From the present PIC simulation, it is also evident that for
electromagnetic field is in the THz frequency range.
shorter laser pulse duration, increase of THz flux and band-
The THz field amplitude and frequency spectrum associ-
width is expected, as the change of asymmetric transient pho-
ated with the radiation are estimated by measuring electric
tocurrent is sharper and the efficiency of THz generation for
field as a function of time at a fixed point in the simulation
a fixed laser wavelength is higher. Moreover, contrary to the
plane. We have measured electric field at a point (50 µm, −50
singl- color case, the dominating factor responsible for THz
µm) far from the central axis so that only the radiated field
radiation is the process of the photocurrent mechanism com-
is taken into account. As can be seen from figure 2, the off-
pared to ponderomotive oscillations. The intense radiation is
axis electric field for the single- and two-color cases cannot be
the consequence of net photocurrent during the propagation of
estimated on the same scale. Electric fields at the fixed posi-
the two-laser pulses in ionized gas.
tion as a function of time are shown in figure  2(e). For the
purpose of comparison, THz emission with the single-color
laser has also been shown. A single cycle of intense radiation 3.  Experimental results
with maximum electric field of 0.58 GV m−1 is observed for
the case ‘θ  =  π/2’. The corresponding THz spectra for gener- Experiments were conducted using 50 femtosecond, 800 nm
ated radiation in both cases is derived by performing Fourier Ti:sapphire laser system delivering horizontally polarized
transform of the line profiles, as displayed in figure 2(e). The laser pulses at 10 Hz repetition rate. A schematic representa-
radiation has a frequency spread to 150 THz, with peak cen- tion of the experimental layout is shown in figure  3. Laser
tered at 40 THz. Notably, figure  2(e) shows the net electric energy is focused using a positive lens to ionize the ambient
field profile of the entire broadband THz radiation rather than air and produce a plasma channel. A 100 µm thick β-barium
a monochromatic one; therefore, the spread of the electric borate (BBO) crystal (type-I) is used for 2ω generation and
field is in time much smaller than the expected in the case of placed between the lens and its focal plane. The fundamen-
nearly monochromatic or narrowband THz radiation (e.g. 1 tal and second-harmonic lasers are co-focused in this way to
THz  ≈  300 µm in space). produce a net asymmetric electric field in the plasma. The
It is important to note that the phase between the funda- plasma channel emits electromagnetic radiation in the THz
mental and second-harmonic fields keeps on changing along frequency range in the forward direction, in a cone [54]. A
the filament length, and also is affected by the plasma dis- pair of 90° off-axis parabolic mirrors (OAPMs) is used first to
persion. However, these effects cannot be accounted for in collimate and then re-focus the THz beam. The focal length of
the analytical photocurrent model. We have also performed a both the first and second OAPMs is 152.4 mm. A 1 mm thick
simulation for the case in which both the laser pulses (ω and high-resistance float zone (HRFZ) silicon wafer is used as a
2ω) are in phase, i.e. ‘θ  =  0’. The simulation results, unlike broadband, high-transmission filter for the THz radiation. A
the prediction of the photocurrent model (figure 1(e)), do not pyro-electric detector has been used to collect the total THz
reveal a drastic difference and are close to the experimental flux under different experimental conditions. At a later stage,
findings seen in figure 5(b). The time profile of the THz field while retrieving the THz frequency content, the pyro-electric
and the corresponding spectrum shown in figure  2(f) match detector is replaced with an EOS setup. During the exper­
closely with the previously reported experimental results [32]. imental campaign, the humidity of the ambiance was kept
It can be asserted from the simulation results that the use of within a limit of 35%  ±  3% to minimize its influence.

5
Laser Phys. 30 (2020) 036002
3.1.  Optimization of second-harmonic crystal
Experimentally, the introduction of 2ω is implemented by
placing the SHG crystal in between the lens and its focal plane.
Such an all-in-line arrangement requires azimuthal orienta-
tion of the SHG crystal, such that the fundamental laser field
has a component parallel to the generated second-harmonic
field. A 2D approach to the photocurrent model incorporates
the experimental parameters to better explain the observations
[55].
As can be seen in figure 4, the horizontally polarized Ti:
sapphire laser beam passes through the BBO crystal with
orthogonal electric field components along the ordinary and
extraordinary axes. We denote these directions as  o for ordi-
nary axis and e for extraordinary axis. In a type-I phase-
matching crystal, two photons of ω frequency along the
ordinary axis combine to generate a 2ω photon in the extraor-
dinary direction. The electric field vector of 800 nm along
the ordinary axis shall contribute to SHG and the orthogonal
component along the extraordinary axis combines with 2ω to
result in an asymmetric electric field in that direction. This
implies a non-zero net current across the extraordinary axis
on a time scale of the driver pulses, and this transient cur­
rent is responsible for THz generation. Net electric field at
the focus of the lens due to fundamental and second-harmonic
laser radiation is given by
EL = Eωe cos (ωt) ê + Eωo cos (ωt + ϕ) ô + E2ω cos (2ωt + θ) ê,
(1)
with ϕ = ω (nωe − nωo ) l/c and θ = ω (nω − n2ω ) d/c + θ0.
In the preceding equation, Eωe and E2ω are amplitudes of
the fundamental and second-harmonic laser fields along the
extraordinary axis. Angle ‘θ’ is the phase difference between
Eωe(t) and E2ω(t) after traveling distance ‘d’ from the BBO
crystal surface to plasma at velocities governed by refractive
indices nω and n2ω, and an initial phase difference ‘θ0’. Angle
ϕ is the phase difference between Eωe(t) and Eωo(t) after pass-
ing through the BBO crystal of thickness ‘l’, induced due to
the inequality in nωe and nωo, i.e. refractive indices of BBO
along e and  o axes.
Figure  5(a) illustrates the evolution of THz energy as a
function of azimuthal angle (α) of the BBO crystal. Rotation
of the BBO in a plane perpendicular to the optical axis decides
the polarization direction of 2ω, which is same as the extraor-
dinary axis. It is observed that THz amplitude varies with a
periodicity of ~π/2. A maximum of 20% of the laser energy
can be converted to its second harmonic. In this situation, the
laser electric field for ω is aligned along the ordinary axis and
corresponds to an azimuthal angle value of 90°, but this is not
the condition for maximum THz conversion efficiency. The
THz amplitude is maximum for α  =  55°, where the combina-
tion of the Eωe and E2ω amplitudes is optimized. Figure 5(b)
shows the effect of relative phase ‘θ’ between the fundamen-
tal and second-harmonic laser fields as a function of the dis-
tance ‘d’ from BBO crystal to plasma. In accordance with
the previous reports [55], the THz yield increases quadrati-
cally for decreasing ‘d’ with a superposed periodic oscillatory
modulation. An oscillatory behavior in the direction towards
plasma is explained by dephasing length arising from the air
6
S Saxena et al
Figure 4.  Vector diagram showing components of horizontally
polarized laser along the ordinary and extraordinary axes of the
BBO crystal.
dispersion. The definition of ‘θ’ from equation (1) implies that
the dephasing length for the THz wave (0  ⩽  θ  ⩽  π) is given by
ld  =  λ/2 (nω  −  n2ω), where λ is the pump laser wavelength, i.e.
800 nm. Periodicity measured from the experiment is 22 mm.
For plasma electron density of ~1016 cm−3 in ambient air
density of ~1019 cm−3, the dephasing length at λ  =  800 nm is
22 mm [56]. The results obtained in this study match closely
with those reported earlier [55].
3.2.  THz flux dependence on laser energy
The THz energy scaling is examined using a  +65 cm focal
length positive lens for focusing laser energy. The laser energy
is controlled by a combination of half-wave plate and polar-
izer. This way any, variation due to the addition of a new optics
in the experimental setup is avoided. As can be seen from
figure  6, the THz energy rises with increasing laser energy.
However, the rate of rise is found to be non-uniform. Unlike
earlier studies where saturation of THz flux is observed with
the laser energy [45], here we observed a jump in the THz flux
beyond certain laser energy. The conversion efficiencies mea-
sured for figure 6 are  >10−4, and the maximum THz energy
obtained during this experiment is 11.2 µJ.
Various reports on THz flux saturation with laser energy
have been published, and the underlying reason stated is
intensity clamping and THz energy reabsorption in plasmas
formed by high-energy laser [48]. In the current experiment,
scaling of THz with laser has been observed, overcoming the
saturation behavior. The enhancement in conversion efficiency
at higher laser energies can be explained by the ionization
mechanism of the plasma medium through the photocurrent
model itself. THz field, according to the PC model, is directly
proportional to the temporal variation of electron density.
Increase of electron density thereby straightaway translates
into an enhancement of the generated THz flux. To quantify
the THz field and spectrum, numerical simulations take into
account ADK tunneling ionization rate and subsequent elec-
tron motion under laser field. Implementing this ionization
rate for atmospheric nitrogen, the second ionization initializes
at ~6  ×  1014 W cm−2. For 50 fs laser pulse duration and 16
µm focused beam size, this intensity corresponds to 24 mJ
Laser Phys. 30 (2020) 036002 S Saxena et al

Figure 5.  Measured THz energy dependence on (a) azimuthal angle of the SHG crystal (BBO) and (b) its distance from the focal plane of
the lens.

laser energy. A change in slope of the THz flux variation is

observed for higher laser energies. This increase is attributed
to the onset of second ionization of N2 molecules. This feature
has been demonstrated but not explained in earlier reports on
THz scaling in the high-laser-intensity regime [45].
We computed the THz flux for varying laser intensity
through the basic PC model to emulate the observations. We
plotted the electron density evolution with time for four differ-
ent laser energies in figure 7(a). Time ‘t  =  0’ corresponds to
the peak of the laser pulse intensity. It is clearly seen that sec-
ond ionization, observed as a step jump in the electron density,
is absent for 8 and 16 mJ laser energies and starts to appear for
24 mJ laser value. For 32 mJ laser energy, a definite enhance-
ment of the electron density can be noticed due to multiple
ionizations in the atmospheric nitrogen taking place. We can
see from figure 7(b) that initially up to 16–20 mJ laser energy,
the THz energy increase is rather modest. Beyond 24 mJ laser
energy, a sudden change in the slope of THz energy with laser
energy is observed, similar to the experimental graph in fig- Figure 6.  THz energy variation with laser energy.
ure 6. A change of trend in the exper­imental graph occurs at focusing geometry confronted by the natural divergence of the
slightly higher energy than that found from the simulation. laser beam and further aided by ionization (plasma)-induced
We explain this feature by the very process of filamentation. defocusing. The dynamic balance of these counteroperating
Ionization of the medium initiates much before the maximum factors leads to propagation of the laser beam much beyond
intensity is attained. Plasma-induced defocusing does not its Rayleigh range determined by its external focusing geom-
allow the filament to reach its minimum focal spot. etry, avoiding localized sharp intensity rise and distributing
To explore the THz flux relation with focusing geometry, the energy over a greater length. In conditions of high laser
the transverse plasma fluorescence is also recorded and ana- energy and short focal-length lens, ionization-induced defo-
lyzed. Figure  8(a) shows images of plasma channel formed cusing is strong. Thereby, tight focusing geometries lead to
at selected laser energy values. Though not an exact meas- ineffective coupling of laser energy into the plasma filament
urement of the electron density evolution, filament image and therefore smaller conversion to THz flux. This phenom­
analysis helps to find an estimate of the laser propagation and enon is also known as intensity clamping in the plasma chan-
energy distribution along the channel. It is known that for nel [57, 58].
low laser energies, the filamentation occurs close to the geo- In figure 8(b), it is clearly seen that for lower laser energy,
metrical focal plane of lens. Increasing laser energy, however, the filament is brightest at far distance along the laser direc-
leads to early onset of ionization. The filamentary propaga- tion. In contrast, a major portion of the energy content is
tion can be considered as interplay between the Kerr effect, dumped earlier into the filament for the higher laser energy. For
which helps in converging the beam, along with its external 40 mJ laser energy, the focusing, defocusing, and refocusing

7
Laser Phys. 30 (2020) 036002 S Saxena et al

Figure 7.  (a) Electron density evolution with time and (b) THz flux computed from the PC model for high-laser-intensity regime.

Figure 8.  Filament image analysis. (a) Transverse images of plasma channel formation for various laser energies. (b) Horizontal intensity
profiles through the filament images exhibiting the laser energy distribution along the length and maximum intensity position. (c) Plasma
volume estimated from FWHM values of the horizontal and vertical intensity profiles. The directional arrows in (a) and (b) indicate the
laser direction.

are clearly seen, distributing the energy content over a much
longer length. We calculated the horizontal and vertical
FWHM length for the filament images captured at varying
laser energies. As is evident from figure 8(c), graph of plasma
volume (πw20 l ) against laser energy matches very closely to
the THz flux as a function of laser energy. Correlation of THz
flux with the plasma volume is well reported [59]. Results
obtained from the analytical simulations, based on the PC
model and image analysis, are in good agreement with each
other. Direct calculation of the electron density at different
laser energies and the indirect measurement through plasma
fluorescence support the proposition that ionization level
increases for higher laser energies and is the reason for the
observed enhancement in THz flux.
3.3.  Effect of apertured laser beam on THz generation
Enhancement in THz flux with apertured pump laser is pre-
sented in this section. As shown in figure, a variable metallic
iris aperture is placed in the collimated laser beam. A con-
verging lens of 65 cm is used to focus laser energy through
the BBO crystal. The input laser beam diameter is 40 mm;
however, the maximum diameter of the aperture is 70 mm.
Unapertured laser energy is pumped into the bi-chromatic
plasma excitation of air medium. Relative humidity during the
experiment was 30%. As can be seen in figure 9, a maximum
of 19 µJ THz energy was observed for an aperture diameter
of 30 mm and laser energy of 31.2 mJ. Maximum conversion
efficiency of ~0.03% observed in section  A (Effect of laser
energy on THz flux) of this paper rose to 0.063% because of
the aperture-limited laser.
THz energy first increases for an increase in the clear area
through aperture, and then falls almost linearly. Varying the
opening of the circular iris aperture has a direct effect on
the spot size, Rayleigh range, transmitted laser energy, and
thereby intensity in the laser plasma core. Focal spot diameter
for the Gaussian beam is defined by w0  =  1.22f λ/D, where
f  is focal length of the converging optics, λ is the laser cen-
tral wavelength, and D is the beam diameter. Plasma channel
cross-section, therefore, increases with the reduction in aper-
ture diameter. Similarly, Rayleigh range for Gaussian beam,
defined as ZR  =  πnw20 /λ , where n is the medium refractive
index, also increases for smaller beam diameters. Truncation
of laser beam therefore translates as increment of the plasma
volume. Enhancement of THz flux observed in figure 9 is a
result of balancing of the two contrasting effects. Reducing
the aperture diameter in incremental steps leads to increas-
ing plasma volume on the one hand and diminishing laser

8
Laser Phys. 30 (2020) 036002
Figure 9.  THz energy as a function of aperture diameter. As the
pump laser energy varies with aperture opening, it has been shown
on the top axis.
Figure 10.  THz flux variation with focal length of the converging
lens.
energy on the other. Peng et al have reported THz enhance-
ment with aperture-limited pump laser, conducted for smaller
beam diameter and much lower laser energy [60]. They have
reported maximum increase in THz flux for 7.5 mJ laser
energy blocked to ~1 mJ value through a 5 mm aperture.
3.4.  THz energy as a function of lens focal length
In another set of experiments, the effect of external focus-
ing geometry on the THz emission from dual-frequency exci-
tation of the ambient air medium is investigated. A 40 mm
laser beam of 50 fs pulse duration and 8 mJ energy is focused
through positive lenses of different focal lengths. The mea-
surements in this study are conducted with He-cooled bolom-
eter having a HDPE filter mounted just before its 10 mm
active area. Several reports have demonstrated through
experiments and simulations that with sufficient laser energy,
9
S Saxena et al
longer-focal-length lenses generate larger THz flux [37, 61].
We conducted the experiment with 20, 30, 40, 50, and 70 cm
focal length lenses. BBO position for each focal length was
initially adjusted for THz generation. Optimum BBO dis-
tance from lens focal plane values for 20, 30, 40, 50, and
70 cm focal length lenses were 6.5, 8.5, 10, 12, and 18 cm,
respectively. This exercise was performed to ensure full illu-
mination of BBO crystal. Optimum azimuthal angle of the
SHG crystal remained the same for varying focal lengths.
As can be seen from figure  10, THz energy rises with
increase in the lens focal length. Difference in THz flux val-
ues from other results is attributed to difference in collection
geometry, humidity level, and spectral selection from the
HDPE filter. Tight focusing geometry causes the formation of
a saturated, bright portion in the filament, promoting inten-
sity clamping and stronger plasma-defocusing effect [57, 58].
Ionization induced defocusing further reduces the plasma
volume, which is the effective source size. The most pri-
mary factor governing the plasma filament length is Rayleigh
range, which is shorter for small focal lengths. Tight focus-
ing therefore restricts effective coupling of laser energy into
plasma, which results in less THz emission. Weak focusing,
on the other hand, supports the formation of a longer plasma
channel and better laser to THz energy conversion. As men-
tioned earlier, dynamic interplay of the Kerr effect and plasma
defocusing in the case of long focal length elongates the fila-
ment length from that governed by the Rayleigh range alone.
The effect of plasma volume has been asserted by reported
experiments [45, 56], where the contribution to THz flux was
restricted by a small aperture moved across the plasma chan-
nel length. All the THz radiation emitted before the aperture is
blocked, and contribution from the plasma length in front was
recorded. The condition where the aperture was placed at the
beginning of the filament along the laser direction resulted in
maximum THz flux. Longer filament lengths support greater
laser to THz conversion efficiency, even for plasma channels
much longer than the dephasing length of fundamental and
second-harmonic lasers due to air dispersion. Off-axis phase
matching of THz radiation has been attributed for such obser-
vations [56].
3.5.  THz beam divergence as a function of lens focal length
It has been observed in experiments [54, 62, 63] that the THz
beam emitted from two-color laser plasma source possess an
inherent divergence with a hollow central part. Though several
theoretical attempts have been made to explain this behavior,
recently You et al [56] proposed the theory of off-axis phase
matching for THz radiation. This was further rigorously inves-
tigated by Gorodetsky et al [64] with detailed numerical mod-
eling including the overdense plasma formation at the core
of the filament and back reflection of THz frequencies. They
demonstrated that the phase matching for THz radiation can
occur only along the off-axis direction, and the angle of diver-
gence is also dependent on the THz frequency [63].
Therefore, for a quantitative comparison of the THz beam
size, radial knife-edge measurement is conducted [65]. A
Laser Phys. 30 (2020) 036002 S Saxena et al

Figure 11.  (a) THz beam size for different focal lengths of the converging lens. Inset of (a) shows a typical pattern of the increment of THz
energy with aperture diameter. (b) FWHM values of the THz beam size have been plotted with respect to the lens focal length. Inset of (b)
is the table of full-angle THz divergence for each focal length studied.

variable metallic iris is inserted in the collimated THz beam

after the first OAPM. The iris aperture is varied by a fixed
amount in each step, and the THz energy is measured after
being refocused by the second OAPM. The THz energy
increases with increasing iris aperture and then reaches a con-
stant value. The constant THz flux for larger aperture opening
signifies that most of the THz emission has been collected.
Figure 11 summarizes the results of the THz divergence
measurements conducted for various focal length lenses.
THz flux for all the focal length lenses rises with increasing
aperture diameter similar to the graph shown in the inset of
figure  11(a). Differentiating this data with respect to length
gives the THz beam extent. It is important to note that from
this measurement, the THz beam size is acquired and not the
exact beam profile. From this approach, the intensity distri-
Figure 12.  Knife-edge measurement of the THz focal spot.
bution within the THz spatial profile cannot be determined
as at each step, integrated transmitted THz flux is recorded. geometry using parabolic mirrors alone can be challenging.
Figure 11(a) signifies that width of the THz beam reduces for To minimize the focused spot radius in such condition, one
increasing focal length. FWHM of the THz beam extent as a should collect the THz radiation with axicon lens or mirror,
function of focal length has been plotted in figure 11(b). THz and then focus with the parabolic mirror [45].
radiation was allowed to diverge for 152.4 mm (focal length of
first OAPM) before being collimated. Half-angle divergence
3.6.  THz focal spot measurement
formed from the center of filament (optic axis) is measured
using half the FWHM value. THz divergence full angles for For a qualitative estimate of the focused THz beam, knife-
each focal length studied have been calculated and inserted in edge measurement is conducted in the focal plane of the
table form in the inset of figure 11(b). The observed values of second OAPM. This is a known technique for beam size esti-
divergence are well within the range of those reported earlier mation [66]. Focal lengths of the collimating and refocusing
for similar focal lengths [59]. It is inferred from this study parabolic mirrors in this study are same, i.e. 152.4 mm. This
that longer-focal-length lenses create a more directional THz ensures that no scaling factor is involved due to the focusing
beam. geometry. A sharp blade is mounted on a horizontal, transla-
An optimization of focusing geometry is therefore required tion stage and moved perpendicular to the laser direction in
for the available laser energy. It was also observed that when the focal plane of the second OAPM. In the initial position, no
the focal length of lens is too long for a given laser energy, THz flux is allowed to reach the detector. As the blade is incre-
a very weak plasma is generated, again resulting in lower mentally shifted, the detector starts showing some THz flux.
than the maximum achievable THz flux. It is also noteworthy The THz detector reading increases gradually and saturates,
that the focused THz spot size is proportional to the filament signifying a fully clear passage for the THz beam. This data
length [56]. Therefore, for applications requiring high THz is the integrated THz energy for the allowed part of the THz
intensity, refocusing the beam generated with weak focusing beam at each position. Therefore, to find the THz focal extent,

10
Laser Phys. 30 (2020) 036002 S Saxena et al

Figure 13.  Experimental setup for electro-optic detection of THz waveform.

Figure 14.  (a) THz electric field as a function of time and (b) THz spectrum as measured by the EOS technique.

this graph is differentiated with respect to length. As seen in
figure 12, the THz beam was focused to a minimum spot size
of 1.94 mm (FWHM).
3.7.  THz spectrum measurement through EOS
EOS is implemented for temporal and spectral characteriza-
tion of the THz radiation generated [67]. A schematic diagram
of the experimental setup implementing the EOS detection
is shown in figure 13. 1% of the horizontally polarized laser
energy is reflected from the surface of a 2° wedge, and is used
as probe. A major part of the laser energy is used as a pump
in the THz generation through two-color laser filamentation
in ambient air. A motorized delay stage in the probe path is
aligned for temporal scanning of probe pulse through the THz
electric field transient. A quarter-wave plate (λ/4) is placed in
the probe path for improvement of signal-to-noise ratio. The
collimated probe is reflected from the surface of a HRFZ-Si
filter, and is co-focused along with the THz beam on surface
of 200 µm thick ZnTe 〈1 1 0〉 crystal. Electro-optic crystals
acquire birefringence in the presence of low-frequency THz
electric field, which is experienced by the femtosecond laser
pulse passing through the crystal. The polarization-modulated
probe laser is collimated through a lens and through the Glan–
Thompson prism, and orthogonal polarization components
are measured on a balanced photo detector. Ellipticity modu-
lation of the probe laser is in this way polarization-analyzed to
provide amplitude and phase information of the THz electric
field.
The motorized stage was translated in steps of 20 µm,
and 26 ps scan was recorded. THz Spectrum is obtained by
performing Fourier transform of the temporal THz profile.
Maximum THz frequency detected using the EOS method is
restricted by the bandwidth support of the crystal. In our case,
ZnTe can faithfully measure spectral count of the THz wave
up to 4 THz [68]. This upper limit is governed by the phase-
matching condition of the optical group velocity with the THz
phase velocity in the crystal. THz pulse duration is found to be
368 fs, as can be seen from figure 14.
4. Conclusion
It can be inferred from our results that THz generation from
two-color laser-induced air plasma is dependent on a number

11
Laser Phys. 30 (2020) 036002
of parameters. We have discussed the factors affecting optim­
ization of the experimental setup for maximal laser to THz
energy conversion. Phase and polarization of the second-
harmonic laser field are controlled by the azimuthal angle of
the second-harmonic crystal and its distance from the focal
plane, respectively. As can be predicted from the photocurrent
model, THz flux maximizes at SH crystal positions separated
by the dephasing length for fundamental and second-har-
monic fields. Scaling of THz flux with laser energy beyond
the saturation region has been demonstrated and explained
by the multiple ionization of the gas medium. Analytical
simulation based on the photocurrent model has been suc-
cessfully used to support this proposition. Estimated plasma
volume from the transverse image of the filament follows a
similar trend as the THz flux with laser energy. The effect of
external focusing geometry is examined by first changing the
input beam size and second, by employing lenses of different
focal lengths. Smaller beam diameter supports larger plasma
volume, in which more laser energy can be coupled. 19 µJ
THz energy was obtained by 30 mm beam diameter, which
is 43% smaller beam size and 22% lesser energy than for the
40 mm full aperture case, in which a 40 mJ laser generates
11 µJ THz. It is inferred from the several parametric stud-
ies reported in this paper that the non-linear phenomenon of
filamentation plays a very important role in the generation
of THz from two-color laser-induced air plasma. Focusing
geometries favoring longer and broader filamentation also
support generation of stronger THz flux. Longer-focal-length
lenses produce greater THz energy, and the resulting THz
beam is smaller in the spatial extent. Focal spot size mea-
surement and temporal field determination by electro-optic
sampling have been presented. For the maximum observed
THz energy of 19 µJ, focal spot diameter of 1.94 mm size,
and pulse duration of 368 fs, a strong THz field of 1.12 MV
cm−1 has been achieved. It should be noted that the pulse
duration measured by electro-optic sampling is much larger
than the actual value, as the ZnTe crystal does not transmit
the majority portion of the broadband THz spectrum gener-
ated from the two-color laser-induced air plasma. The THz
radiation from this source can effectively be used for non-lin-
ear THz spectroscopy and other applications requiring large
THz flux. The photocurrent model has been explained, and
analytical simulations based on it are employed to justify the
experimental findings reasonably well. The results of the 2D
PIC simulation have been reported and the role of transient
photocurrent in THz generation has been well asserted.
Acknowledgments
The authors (SS, SB, BSR and JAC) thank R A Joshi, R K
Bhat for laser operations and S Sebastin, L Kisku, K C Par-
mar for providing ground support during the experimental
campaign. SK and DNG thank the Department of Physics and
Astrophysics, University of Delhi, for providing the facility of
high performance cluster machine to carry out the simulation
work.
12
S Saxena et al
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