Jewariya et al. Vol. 26, No. 9 / September 2009 / J. Opt. Soc. Am.

B A101

Enhancement of terahertz wave generation by

cascaded ␹„2… processes in LiNbO3

Mukesh Jewariya,1,* Masaya Nagai,1,2 and Koichiro Tanaka1,3

1
Department of Physics, Kyoto University, Kyoto 6068502, Japan
2
Precursory Research for Embryonic Science and Technology (PRESTO),
Japan Science and Technology Agency (JST), Japan
3
Institute for Integrated Cell-Material Science (iCeMS), Kyoto University, Kyoto 6068501, Japan
*Corresponding author: [Link]@[Link]

Received February 4, 2009; revised May 21, 2009; accepted June 5, 2009;
posted June 9, 2009 (Doc. ID 107170); published July 20, 2009
We demonstrate, to the best of our knowledge, a novel generation process of a terahertz (THz) electromagnetic
wave via a noncollinear ␹共2兲 process in LiNbO3 with a phase-front-controlled femtosecond Ti:sapphire laser
pulse. Systematic measurements of both the THz electric field and the excitation transmitted through an
LiNbO3 crystal at different excitation powers show that the maximum amplitude of the THz electric field in-
creases nonlinearly above the critical input powers. This enhancement of optical rectification efficiency is at-
tributed to the distortion of the excitation pulse shape via electro-optic (EO) phase modulation by the emitted
THz wave. Actually, spectral line shapes of both the THz wave and the excitation pulse become broadened
above the threshold, and they are well reproduced by numerical simulations with equivalent one-
dimensionally mapped coupled equations in the frequency domain. This generation scheme shows potential
optimization of further generation efficiency. © 2009 Optical Society of America
OCIS codes: 190.4410, 040.2235.

1. INTRODUCTION dition is not satisfied in simple collinear geometry, so non-

Resonances lying in THz frequency region such as inter- collinear excitation geometry [8] or periodic pole LiNbO3
molecular vibration mode, gap in superconductors, soft- [9,10] is used for nanosecond pulse excitation. Recently,
mode in dielectrics, and magnetic resonance govern coop- Hebling et al. demonstrated intense THz wave generation
erative phenomena of materials, attracting the material using a tilted wavefront technique [11,12]. Pulse-front
scientists. The recent development of ultrafast optical tilting of the ultrashort excitation pulse permits phase
pulse techniques resulted in the efficient generation and matching in the direction of THz wave propagation, even
detection technique of the coherent THz pulse in the time for broadband pulse excitation. They used grating and
domain, which allows us to access resonances with high lenses for controlling lateral dispersion of the excitation
accuracy [1,2]. The electric field obtained with time- wave packet [13] and simultaneously controlled spectral
domain spectroscopy, both the amplitude and the phase angular dispersion matched to the phase matching condi-
with a wide frequency region, directly provides much in- tion. With the assumption of differential frequency gen-
formation that is characteristic for material, complex di- eration, the phase matched condition can be satisfied as
electric functions. However, there are several difficulties ng = nTHz cos ␪, where ng is the visible index of the group
remaining when one reveals these resonances, because a velocity, nTHz is the THz index of phase velocity, and ␪ is
spectral overlap of the resonances prevents it from reveal- the angle between optical and THz beams. A record out-
ing details of material dynamics in the THz frequency re- put power of a THz pulse is 10 ␮J using this technique
gion. In looking back in the history of spectroscopy, non- [14], and the conversion efficiency is 5 ⫻ 10−4 [15].
linear spectroscopy, such as photon echo and hole For obtaining higher efficiency THz generation, exact
burning, is crucial for overcoming these difficulties. recognition of the cascaded optical rectification process is
Therefore, a high-power THz light source has been re- crucial. Obeying the Manley–Rowe limit, the energy con-
quired for this purpose. The nonresonant optical rectifica- version rate should be low because of the tiny photon
tion process is one of the most ideal and well-established quantum energy of the THz wave. However, an excitation
methods for THz wave generation because high conver- photon emitting one THz photon beam converts into an
sion efficiency of emitted THz radiation is retained, even optical beam with a small, low-frequency shift. This beam
under significant high-power excitation. Several ␹共2兲 ma- will promote further generation processing of the THz
terials that satisfied collinear phase matching conditions wave if the phase matched condition is satisfied. In prac-
have been characterized for emitters [3–7], and the THz tice, Hebling et al. reported a spectral shift of a transmit-
electric field emitted from these materials is large enough ted excitation beam larger than the weighted frequency of
to perform linear spectroscopy. LiNbO3 has a large ␹共2兲 a THz wave in intense THz wave generation and pointed
value and is a very good candidate for a THz emitter crys- out cascaded optical rectification processes [14]. In these
tal. Due to strong index dispersion, the phase match con- cascaded processes we also focus on the inverse ␹共2兲 pro-

0740-3224/09/09A101-6/$15.00 © 2009 Optical Society of America

A102 J. Opt. Soc. Am. B / Vol. 26, No. 9 / September 2009 Jewariya et al.

cesses corresponding to the EO process. Strong spectral ⫻ 2 mm2. The size of the emitter crystal is 5 ⫻ 5 ⫻ 5 mm3.
modulation of an excitation beam induced by THz wave We use stoichiometric LiNbO3 crystals with low Mg con-
generation indicates the distortion of the excitation pulse centration (1.5%), because reduced Mg doping is still suf-
shape. Self-induced optical phase distortion in EO crys- ficient to prevent photorefractive damage [21]. One sur-
tals was first predicted in GaAs EO crystals and conven- face is cut at an angle of 62° with an antireflection coating
tional YAG lasers [16]. Considering cascaded ␹共2兲 pro- for the near infrared beam. The generated THz pulses are
cesses related to second-harmonic generation processes guided with two off-axis parabolic mirrors, and the emit-
[17], the near phase matching of the cascaded ␹共2兲 process ter’s image is transferred onto the surface of the EO crys-
is important for pulse compression. This noncollinear ge- tal at half size. The other sampling beams of the THz
ometry of excitation with angular frequency dispersion is pulses are also focused on the same spot of an EO crystal
analogous to the pulse compression technique with non- for detection through the small hole of a parabolic mirror,
collinear coherent anti-Stokes Raman scattering [18]. If and the birefringence of the sampling beams modulated
the pulse duration of an excitation pulse is shortened via by the electric field of THz pulses are measured using a
a generated intense THz wave, the conversion efficiency quarter-wave plate, Wolston prism, and two balanced Si
of the THz wave generation is enhanced and the band- detectors. The electric field can be easily calibrated from
width of the THz wave becomes broadened. Recently, we the EO modulated signal. By varying the time delay be-
experimentally demonstrated broadband THz pulse gen- tween a THz pulse and a sampling pulse, the electric field
eration using a Yb-doped fiber laser pulse with a 1.04 ␮m amplitude of THz pulses can be detected as a function of
wavelength and a 600 fs pulse duration [19]. A spectral time. For a high S/N ratio measurement, we synchro-
bandwidth of a THz wave above 2 THz is beyond the limi- nously chop the pump beam at 500 Hz, which blocks ev-
tation of an incident pulse profile because it directly ery alternate pump pulse. After the sampling beam is
shows the inverse of an excitation pulse duration, not the sampled in a boxcar integrator that inverts every electric
bandwidth of an excitation pulse [20]. In this paper, we signal, a computer collects the electric signals and sepa-
systematically measure both the power spectra of a THz rates them to extract EO-modulated signals and non-
wave from an LiNbO3 crystal and the transmitted excita- modulated ones.
tion beam with tilted pulse front excitation using a con- For an EO detector crystal we use a (110)-oriented GaP
ventional Ti:sapphire laser at different excitation powers. crystal with the thickness of L = 0.3 mm. While a phase
Experimental results show that THz wave generation ef- match condition at 800/ 780 nm wavelength is not com-
ficiency is enhanced by excitation pulse distortion via ␹共2兲 pletely satisfied, a low EO coefficient 共r41 = 1 pm/ V兲 and a
cascaded processes. The cascaded ␹共2兲 process in LiNbO3 high phonon frequency make intense and broadband THz
has the potential of further high-efficient THz generation. radiation detectable. An EO signal caused by phase shift ␪
can be easily calibrated with the formula ⌬I / I = sin ␪
= 2␲ / ␭nopt3r41ETHzL, where nopt = 2.85 is the refractive in-
2. EXPERIMENTAL SETUP dex of GaP at ␭ = 800 nm [22]. This detection technique is
available at a low induced electric field. Recall that sensi-
Figure 1 shows the schematic of the experimental setup
tivity becomes saturated when a modulated phase shift
for the THz electric field measurement. We use optical
induced by an intense THz electric field reaches ␲. We put
pulses from an amplified Ti:sapphire laser system with a
four Si plates in the path of THz radiation as attenuation
repetition rate of 1 KHz, an average power of 800 mW, a
filters with large reflection loss and suppress the modu-
central frequency of 800 nm, and a pulse duration of
lated signal. For obtaining a true-time evolution of the
150 fs (full width at half-maximum intensity). The beam
electric field, we compensate for a complex Fourier com-
splits into two beams for THz generation and detection.
ponent of the electric field divided by a sensitivity factor
The tilted angle of the excitation beam is controlled with
of 2 / 共nTHz-1兲 共ei⌬kL-1兲 / i⌬k in GaP determined by Fresnel
an Au-coated 1800/ mm holographic grating and two
loss and phase mismatching ⌬k. Thus we carefully evalu-
lenses and is focused on the emitter with a spot size of 3
ate the spectral line shape of the emitted THz wave at dif-
ferent excitation powers.

3. EXPERIMENTS
Figure 2 shows the temporal evolution of an electric field
evaluated from the EO signal. The electric field in the left
axis is calibrated with Si plate attenuators and phase
mismatching in the GaP detector. The input power per
pulse is 650 ␮J. The time delay between two minimum
signals is 0.9 ps and the calibrated maximum electric
field is 193 KV/ cm, where the maximum magnetic field
for a TEM wave is 670 gauss. From this temporal profile,
we can evaluate the power density of 33 ␮J / cm2 using the
relation ␧0c兰E共t兲2dt. By moving one parabolic mirror in
the direction parallel to the emitter surface, the trans-
Fig. 1. Experimental setup of emitted THz electric field ferred image of the emitter can be moved on the detector
measurement. surface and the horizontal beam distribution of 1.5 mm
Jewariya et al. Vol. 26, No. 9 / September 2009 / J. Opt. Soc. Am. B A103

emitted THz wave. We cool down the emitter to show the

evidence of our theoretical consideration. The absorption
coefficient at room temperature is several tens of cm−1 in
the THz frequency region, but it should be suppressed by
cooling. We control the emitted THz electric field by tem-
perature change, and we can verify whether this super-
linear behavior is related to the emitted THz electric field.
We set the LiNbO3 emitter in a liquid nitrogen cryostat
with a near-infrared antireflection-coated window and a
plastic window transparent in the THz frequency region,
and similar experiments were performed. Due to the limi-
tation of our experiments, we measured the temperature
dependence of THz wave generation with a different am-
plified Ti:sapphire laser system (1 kHz repetition rate,
450 mW output power, 775 nm center wavelength, and
150 fs pulse duration). At low input power, the observed
output electric field at low temperature is 2.2 times larger
than that at room temperature. Since absorption in the
THz frequency region becomes probably less than 1 / 5 by
cooling to 77 K [24], this electric field enhancement is rea-
Fig. 2. Temporal evolution of THz electric field from LiNbO3 sonable. Note here that super-linear behavior is observed
under femtosecond laser excitation. when the output electric field is almost 10 kV/cm. We also
observe sublinear behavior when the output electric filed
can be moved on the surface of the emitter. Thus we is hundreds of kV/cm, so the output electric field at the
evaluate that the output power is 300 nJ per pulse from maximum input power is almost the same as that of the
the EO measurement, which is slightly smaller than the room temperature emitter. It clearly indicates that the ob-
power of 570 nJ measured directly with the pyroelectric served super-linear behavior is related to the emitted THz
detector (SPI-A-62 THz, Spectrum Detector, Inc.). The electric wave.
corresponding conversion efficiency to this power is ac- In general, we treated it using nonlinear coupled equa-
complished at 8 ⫻ 10−4, almost the same as reported in tions [25], indicating that the THz wave is generated by
previous reports [15]. the optical excitation beam, and alternatively, the optical
Figure 3 shows the excitation power dependence of the excitation beam is modulated by the emitted THz wave.
THz electric field. The dotted line shows a slope of 1. Con- Considering zero initial conditions for the THz compo-
sidering the simple optical rectification process, the elec- nent, the THz beam is generated first and the spectrum of
tric field of THz radiation should be proportional to the in- the excitation beam is strongly modulated when the pho-
put power [20]. However, super-linear behavior is ton number of THz wave approaches that of the excitation
observed above the input power of 100 ␮J. Stepanov et al. beam. Actually, Y. Shen et al. experimentally demon-
have reported similar behavior [23] and interpreted it strated that an intense THz electric field can control the
with spatial modulation of the excitation pulse. We con- temporal phase of a weak ultrashort laser pulse copropa-
sider that this is due to optical pulse shape distortion via gating in a ZnTe EO crystal [26]. Consequently, pulse
shape distortions should influence the efficiency of THz
generation.
To confirm this scheme, spectral information of both
the THz wave and the excitation beam is critical. Figure
4(a) shows the power spectra of the emitted THz wave at
room temperature with different excitation powers. The
weighted center frequency of the power spectrum lies at
0.73 THz at low input power, but it shifts to 0.88 THz at
the maximum input power, implying that high-frequency
components are increasing. Actually, this spectral change
becomes obvious above the input power of I0 / 4, which cor-
responds to the thresholds shown in Fig. 3. Therefore, the
enhancement of conversion efficiency originates from the
broadening spectral bandwidth. We also measured the op-
tical spectra of excitation pulses transmitted through the
LiNbO3 crystal because these include complementary in-
formation on divided excitation beams. Figure 4(b) shows
simultaneously measured optical spectra of transmitted
excitation pulses from LiNbO3. The weighted center
wavelength of the excitation beam is 800 nm at low exci-
Fig. 3. Input power dependence of peak electric field of THz tation power. However, spectral shifts toward longer
radiation. Dotted line corresponds to slope of 1. wavelengths proceed above I0 / 4, and the center wave-
A104 J. Opt. Soc. Am. B / Vol. 26, No. 9 / September 2009 Jewariya et al.

Fig. 5. (Color online) Scheme of mapping from (a) the two-

dimensional noncollinear parametric process to (b) a simple one-
dimensional scheme.

the angle of ␪ coincidentally emits toward site b2. In this

situation, the propagation length of the THz wave is
dz / cos ␪, causing corresponding propagation loss of the
Fig. 4. (a) Power spectra of THz radiation from LiNbO3 at dif- THz beam. When we assume the parametric process in
ferent excitation powers. (b) Optical spectra of transmitted exci- the domain of site b2, we use electric fields of the excita-
tation pulses through LiNbO3 at corresponding excitation pow- tion beam from site b1 and THz beam from site a1. The
ers, which includes the information of the signal beam. These
spectra are normalized by their area. point is that the excitation beam from site a2 is basically
equivalent to that from site a1, consequently allowing us
length lies at 815 nm at the maximum power of I0, which to map to the one-dimensional propagation equations
corresponds to a 6 THz frequency shift. coupled between optical electric field E共␻0 + ␻兲 and THz
We evaluate the quantum efficiency of the THz wave electric field E共␻THz兲 derived as

冑
from the spectra in Fig. 3. If a whole optical excitation
dE共␻0 + ␻兲 ␣opt ␮0 共␻0 + ␻兲
pulse converts into a THz wave at a center-weighed fre- =− E共␻0 + ␻兲 − id
quency of 0.88 THz, the expected energy conversion effi- dz 2 ␧0 n共␻0 + ␻兲
ciency is 2.7⫻ 10−3; thus, we evaluate a net quantum effi-
ciency of 0.3 in our experimental scheme. However, the
spectral line shape of the THz wave and transmission
⫻ 冕 E共␻0 + ␻ − ␻THz兲E共␻THz兲exp关i共k共␻0 + ␻兲
shows a quantum efficiency of 6 / 0.88= 6.8. This discrep-
ancy is probably due to the absorption of a high-THz- − k共␻0 + ␻ − ␻THz兲 − k共␻THz兲兲z兴d␻THz
frequency wave in LiNbO3 as well as a Fresnel loss and
steep diffraction from the emitter, and we believe a quan-
tum efficiency of around 1 in our generation scheme.
− id 冑 ␮0 共␻0 + ␻兲
␧0 n共␻0 + ␻兲
冕 E共␻0 + ␻

+ ␻THz兲E*共␻THz兲exp关− i共k共␻0 + ␻ + ␻THz兲

4. PROPAGATION EQUATIONS COUPLED − k共␻0 + ␻兲 − k共␻THz兲兲z兴d␻THz , 共1兲
BETWEEN OPTICAL AND TERAHERTZ

冑
PULSES
In order to understand this nonlinear process in LiNbO3
for its optimization, we generally consider this process
dE*共␻THz兲
dz/cos ␪
=−
␣THz
2
E*共␻THz兲 + id
␮0 ␻THz
␧0 n共␻THz兲
冕 E共␻0

with coupled equations in the frequency domain rather

+ ␻ − ␻THz兲E*共␻THz兲exp关i共k共␻0 + ␻兲 − k共␻0
than in the time domain [12]. Such a simulation has been
performed in a ZnTe THz emitter [27]. For simulation un- + ␻ − ␻THz兲 − k共␻THz兲兲z兴d␻ . 共2兲
der a simple, slowly varying envelope approximation, we
consider both an optical excitation pulse and a THz pulse Here ␣o/THz are absorption coefficients in the optical/THz
as the summation of the frequency components with a frequency regions, d is the nonlinear coefficient, and ␧0
plane wave approximation. We also consider both an op- and ␮0 are the dielectric constant and magnetic permit-
tical excitation pulse and a THz pulse as the summation tivity in vacuum, respectively. The second and third terms
of frequency components with the plane wave approxima- in the right side of Eq. (1) show EO phase modulation by
tion. An incident excitation pulse with a tilted pulse front the THz electric field, and the second term in the right
has given an angular frequency dispersion, so the k vector side of Eq. (2) shows the optical rectification process. Re-
direction of each frequency component, including the THz call that this model based on plane wave approximation
wave, is automatically determined by obeying the k selec- does not include spatial modulation such as self-focusing
tion rule of the ␹共2兲 process. We can simplify one- of the optical pulse or the cascaded ␹共2兲 processes after the
dimensional plane-wave propagation equations, even in long-distance propagation of an optical pulse. But we can
two-dimensional propagation. Figure 5 shows the scheme reproduce characteristic properties of optical and THz
of mapping from a two-dimensional noncollinear para- spectra with even simple equations.
metric process to a simple one-dimensional scheme. We The incident light pulses with a Gaussian profile is de-
assume an optical parametric process during excitation scribed by E共0 , t兲 = E0 exp关−2 ln 2t2 / ␦t2兴exp关−i␻0t兴, where
beam propagation in the small domain near the emitter ␦t is the pulse duration in the Fourier transformed limit.
surface (site a1) with the distance of dz. This excitation The Fourier transformed optical electric field becomes
beam in site a1 passes toward site b1, and THz beam with E共0 , ␻兲 = 共E0␦t / 2冑2␲ ln 2兲exp关−␦t2␻2 / 8 ln 2 − i␤␻2兴. For
Jewariya et al. Vol. 26, No. 9 / September 2009 / J. Opt. Soc. Am. B A105

later simulation including the chirp effect, we add the sec- pulse, and the bandwidth of a THz pulse is narrower than
ond order dispersion term i␤␻2 in this formula. Optical that of an excitation pulse due to strong high-frequency
dispersion of LiNbO3 is used in the visible frequency re- THz absorption in LiNbO3. Additionally, we have to as-
gion [22] and in the THz frequency region [24]. We neglect sume spatial modulation [23] as well as phase modulation
absorption in the visible frequency region. in the time domain, which makes its interpretation com-
Figure 6 shows the simulated spectra of the THz pulse plicated. Recently we reported THz wave generation with
and the transmitted optical pulse. The excitation powers the bandwidth above a 600 fs duration excitation pulse
correspond to those in Figs. 4(a) and 4(b). Considering the [19], which clearly shows pulse compression via the cas-
spectral bandwidth of the THz wave at low excitation caded ␹共2兲 process. Our experiments and simulation
powers in our experiments, the incident excitation beam should support further development of novel THz genera-
seems to have a 200 fs pulse duration, longer than the tion techniques with optical pulse shaping.
original pulse width of 150 fs. This is probably due to
chirping of the excitation pulse being chirped by the grat-
ing and the lens pair. We assume the incidence of the 5. SUMMARY
chirped excitation beam with ␤ = 0.2 rad ps2 in our analy-
In conclusion, we demonstrate the enhancement of THz
sis. Transmitted excitation spectra in the simulation are
wave generation in an LiNbO3 crystal by cascaded ␹共2兲
superposed with various propagation lengths because
processes. An intense THz electric field generated by op-
noncollinear configuration causes excitation pulses pass-
tical rectification in an LiNbO3 crystal induces phase
ing through the different propagation lengths in LiNbO3.
modulation in the optical excitation pulse, resulting in ex-
One can see that a broadening of the excitation beam to-
citation pulse distortion, which brings in highly efficient
ward the low-frequency region occurs above the excitation
broadband THz wave generation. Experimental results
density of I0 / 8 with a periodic spectral line shape. The
using a Ti:sapphire laser are successfully reproduced by
bandwidth of the THz wave also becomes broadened, co-
numerical simulation with a one-dimensionally mapped
incidently. This spectral change is relatively smaller than
coupled equation. This enhancement of THz wave genera-
the spectrum of the excitation pulse because enhanced
tion via the cascaded ␹共2兲 process is brought out more by
high-frequency THz components are strongly absorbed in
subpicosecond pulses and should be crucial for the design
LiNbO3. These features are successfully reproduced by
of future THz light sources.
the experimental results as shown in Fig. 4, which indi-
cates that the enhancement of THz wave generation is at-
tributed to the cascaded ␹共2兲 process.
Pulse distortion via the cascaded ␹共2兲 process has the ACKNOWLEDGMENTS
potential of optical pulse compression. Shen et al. re- The authors acknowledge a Grant-in-Aid for the global
ported pulse distortion via an external THz electric field COE “The Next Generation of Physics, Spun from Univer-
modulation in an EO crystal [26] and implied that pulse sality and Emergence” and a Grant-in-Aid for Creative
compression may be possible with some adjusted time de- Scientific Research grant 18GS0208 from the Ministry of
lay between THz and optical pulses. However, we cannot Education, Culture, Sports, Science, and Technology
verify it clearly from our experimental results. We can (MEXT) of Japan.
imagine a temporal profile of excitation pulses with any
chirping from the THz wave spectrum because the pulse
duration directly reflects the THz bandwidth [20], and we
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