Research Article Vol. 31, No.

22 / 23 Oct 2023 / Optics Express 36410

Sub-picosecond tunable mid-infrared light

source for driving high-efficiency optical
rectification
J INSHENG L IU , 1,2,† Y UFANG D ING , 1,† X INGBIN G U , 1,† P ENG
Y UAN , 1 D ONGFANG Z HANG , 1 J ING WANG , 1 G UOQIANG X IE , 1
H ENG T U , 3 J IYONG YAO, 3 L IEJIA Q IAN , 1,4 AND J INGUI M A 1,*
1 Key Laboratory for Laser Plasmas (MOE), Collaborative Innovation Center of IFSA (CICIFSA), School of
Physics and Astronomy, Shanghai Jiao Tong University, Shanghai 200240, China
2 Shanghai Institute of Laser Plasma, China Academy of Engineering Physics, Shanghai 201800, China
3 Key Laboratory of Functional Crystals and Laser Technology, Technical Institute of Physics and
Chemistry, Chinese Academy of Sciences, Beijing 100190, China
4 Tsung-Dao Lee Institute, Shanghai Jiao Tong University, Shanghai 200240, China
† These authors contributed equally to this work.
* majg@sjtu.edu.cn

Abstract: Optical rectification (OR) is a popular way to generate coherent terahertz radiation.
Here, we develop a sub-picosecond mid-infrared (mid-IR) light source with a tailored wavelength
and pulse duration for enhancing the OR efficiency. Numerical simulations for a LiNbO3 -based
OR with tilted pulse-front excitation are first conducted to determine the optimal parameters of
pump wavelength and pulse duration, demonstrating that the OR efficiency pumped by 4-µm
sub-picosecond (0.5-0.6 ps) pulses is approximately twice the value with 0.8-µm pump at the
same conditions. Guided by the simulation results, we build a BaGa4 Se7 -based optical parametric
chirped-pulse amplification system with 1030-nm thin-disk pump and broadband mid-IR seeds.
The output performances of >200-µJ pulse energy, ∼600-fs pulse duration and 1-kHz pulse
repetition rate are achieved in a spectral range tunable from 3.5 to 5 µm. The large energy
scalability and high parameter tunability make the light source attractive to high-efficiency OR in
various materials.

© 2023 Optica Publishing Group under the terms of the Optica Open Access Publishing Agreement

1. Introduction
Since its invention, the laser has not only revolutionized scientific research, medical treatment,
and industrial processing, but also given birth to various secondary radiation from X-rays to
terahertz (THz) waves via nonlinear optical effect or laser-plasma interaction. The laser for
driving nonlinear or strong-field processes is characterized by ultrashort pulse duration and
ultrahigh peak intensity. At present, such ultrashort intense lasers mainly distribute in the
near-infrared (near-IR) region, where the involved materials and technologies are well-developed
[1]. The most popular 800-nm Ti:sapphire regenerative amplifiers, integrating the technologies
of Kerr-lens mode-locking and chirped-pulse amplification in broadband Ti:sapphire crystals,
can offer ultrashort pulse duration below 30 fs, gigawatt-to-terawatt peak power, 1-kHz pulse
repetition rate, and controllable carrier-envelop phase. With Ti:sapphire lasers, radiations with
much shorter or longer wavelengths can be generated via nonlinear frequency conversion. For
instance, Ti:sapphire-laser-pumped high-order harmonic generation (HHG) can produce extreme
ultraviolet radiations with a cutoff energy of ∼ 100 eV [2,3]; and as for longer wavelengths,
Ti:sapphire-laser-pumped optical rectification (OR) can radiate coherent terahertz pulses [4,5].
The rapid development of the above strong-field and nonlinear processes puts forward higher
requirements on the pump sources [6], which is beyond the power of Ti:sapphire laser. For the
HHG, the cutoff energy of the harmonic spectrum depends on the product of the driving laser

#504548 https://doi.org/10.1364/OE.504548
Journal © 2023 Received 30 Aug 2023; revised 2 Oct 2023; accepted 5 Oct 2023; published 13 Oct 2023
 Research Article Vol. 31, No. 22 / 23 Oct 2023 / Optics Express 36411

intensity and the square of the wavelength [7,8]. As the laser intensity is limited by ionization,
the increase in driving wavelength proves to be a valid approach for boosting the cutoff energy.
Therefore, mid-infrared (mid-IR) ultrafast intense lasers are drawing more and more attention.
Optical parametric chirped-pulse amplification (OPCPA) is now the workhorse to generate
few-cycle intense laser in the mid-IR region [9–13]. With the aid of a 3.9-µm OPCPA source, for
example, up to 5001 harmonics have been generated [7] and the cutoff energy has reached hard
X-ray region [8].
In addition to HHG, OR also addresses a strong quest for a mid-IR driving source. With
traditional Ti:sapphire lasers, the multi-photon absorption of crystals on pump pulses will limit
the conversion efficiency from laser to THz in OR [14]. For the commonly used LiNbO3
materials, its bandgap of ∼3.9 eV is smaller than triple the 800-nm photon energy (∼1.55 eV),
so three-photon absorption dominates at high-intensity pump, which hampers the increase of
efficiency with pump intensity and even degrades the damage threshold of the materials. The
reported efficiencies of Ti:sapphire-laser pumped OR in LiNbO3 are typically 0.1-0.7% at room
temperature [15,16], and 1.2% with cryogenic cooling [5], depending on pump fluence. Recently,
it has been demonstrated that mid-IR laser pump can help increase the conversion efficiency of
OR by suppressing the multi-photon absorption [17,18]; with a 2-µm pump source, a record
laser-to-THz conversion efficiency approaching 6% has been achieved in an organic material
DAST [17]. However, there are few reports for the efficiency improvement of LiNbO3 -based OR
by mid-IR excitation.
For OR, another key problem is that there lacks a pump source specifically customized for
it. The development of a laser system usually pursues shorter pulse duration for increasing the
peak power. However, the pulse duration is not the shorter, the better for OR [19]. Simulations
and experiments prove that the optimal pulse duration for OR in LiNbO3 is 350-750 fs under a
near-IR laser pump [20–23], which is required to be a Fourier-transform-limited (FTL) pulse
rather than a chirped pulse. This is understandable because one cycle of a 1-THz pulse is 1 ps;
and the useless spectral components within a much shorter pump pulse will lower the conversion
efficiency of OR [19].
In this study, we develop a mid-IR sub-picosecond high-repetition-rate light source tailored for
OR, which is built by three-stage OPCPA with BaGa4 Se7 (BGSe) crystals pumped by a Yb:YAG
thin-disk laser. The BGSe crystal with a broad transmission spectrum covering 0.47-18 µm can
support bandwidth-limited but tunable phase matching (PM) in the range of 3-8 µm, allowing the
direct generation of FTL sub-picosecond mid-IR lasers. Based on a ready-made broadband seed
source, the OPCPA system can output >200 µJ pulse energy in a spectral range tunable from 3.5
to 5 µm, which matches the transparent range of LiNbO3 . The compressed pulse duration of ∼
600 fs adapts to the predicted optimal pulse duration for LiNbO3 -based OR. To the best of our
knowledge, this is the first mid-IR OPCPA based on BGSe crystals and the first mid-IR light
source specifically developed for driving high-efficiency OR.

2. Efficient optical rectification driven by mid-IR laser

Prior to system description, numerical simulations are first conducted to explore the dependence
of OR efficiency on the wavelength and duration of pump pulses. The simulations are based on a
conventional OR scheme in LiNbO3 prism with tilted-pulse-front (TPF) pumping [24], as shown
in Supplement 1. A diffraction grating induces angular dispersion onto the pump pulse, leading
to a TPF in the LiNbO3 crystal to realize a noncollinear PM between the pump pulse and THz
radiation. The required TPF angle varies with the pump wavelength. To highlight the effect of
wavelength and pulse duration on the efficiency, here the pump fluence is kept at 200 mJ/cm2
for all cases although a higher fluence is allowed for the long-wavelength pumping. In each
case, the pump-to-THz efficiency refers to the peak efficiency along the interaction length within
 Research Article Vol. 31, No. 22 / 23 Oct 2023 / Optics Express 36412

the crystal. All cases share the same grating and imaging optics and the detailed simulations
parameters are given in the Supplement 1.

Fig. 1. Simulation results on optical rectification (OR) in LiNbO3 prism with tilted-pulse-
front pumping at both room temperature of 300 K (blue) and cryogenic cooling of 80 K
(yellow). (a) Pump-to-THz efficiency versus the pump wavelength. The pump pulses have the
same Fourier-transformation-limited (FTL) duration of 500 fs. (b) Pump-to-THz efficiency
versus the FTL pulse duration of a 4-µm pump pulse. (c) Pump-to-THz efficiency versus the
interaction length, with a pump wavelength of 4 µm and a FTL pulse duration of 600 fs. (d)
THz spectra corresponding to efficiency peaks in Fig. 1(c). Please refer to the Supplement 1
for detailed simulation parameters.

The dependence of pump-to-THz efficiency on the pump wavelength is simulated first, as

shown in Fig. 1(a). The pump wavelength is tuned from 0.8 to 4 µm and the cases beyond 4 µm are
not calculated considering the LiNbO3 absorption. All the pump pulses are assumed to have the
same FTL duration of 500 fs. In our simulation code, the crystal absorption on THz radiation is
considered, so the simulations are conducted at two temperature levels. At the room temperature
of 300 K, the efficiency increases with the pump wavelength, which is 0.35% at 800-nm pump
and increases to beyond 1% at 4-µm pump [blue curve in Fig. 1(a)]. The simulation results show
the advantage of mid-IR laser pump on enhancing the efficiency of OR. The efficiencies can be
further enhanced by lowering the temperature as the crystal absorption on THz wave decreases
with temperature. At cryogenic cooling of 80 K [yellow curve in Fig. 1(a)], the efficiencies greatly
exceed the corresponding values obtained at room temperature; for example, the efficiency of
 Research Article Vol. 31, No. 22 / 23 Oct 2023 / Optics Express 36413

the 4-µm pump case reaches 1.6% at 80 K. Note again that above efficiencies are calculated at
the same pump fluence for all the pump wavelengths. In practice, the mid-IR pump fluence
can be higher due to the less three-photon absorption and higher damage threshold, so a higher
efficiency is expected at the mid-IR pump.
Next, the effect of the FTL pump pulse duration on OR efficiency is studied at the pump
wavelength of 4 µm [Fig. 1(b)]. The pump duration is tuned from 0.1 to 1 ps while the pump
fluence remains constant. Initially, increasing the pump pulse duration from the commonly used
100 fs results in a significant increase in the pump-to-THz conversion efficiency. The efficiency
arrives at a peak when the pump duration is ∼600 fs. After the peak, the efficiency begins
decreasing with the pump duration. Therefore, the optimal choice of pump pulse duration is ∼
600 fs under the calculation conditions with a minor change when the temperature degrades from
300 to 80 K. For shorter FTL pulse duration, the effective interaction length between the pump
and THz pulses is small, which limits the THz yield. For longer FTL pulse duration, the lower
pump intensity results in a slow growth of THz, which is susceptible to crystal absorption. As
the OR can be regarded as an intra-pulse difference frequency generation (DFG) in the frequency
domain, simply chirping a short pump pulse to reach the optimal pulse duration is ineffective for
optimizing the efficiency.
Under the 4-µm pump with an optimal FTL pulse duration of 600 fs, the efficiency evolution
with the interaction length is given in Fig. 1(c). The efficiency increases first, enters saturation
then, and decreases finally due to the onset of crystal absorption. The efficiency peak occurs
at the interaction length of ∼1 mm at 300 K and ∼1.1 mm at 80 K, where the corresponding
THz spectra are plotted in Fig. 1(d). The THz spectrum at 80 K contains more high-frequency
components due to less absorption at low temperature.

3. System design and experiment setup

From the above simulations, the high-efficiency OR calls for a tunable mid-IR light source with
sub-picosecond FTL pulse duration. To satisfy these requirements, we try to adopt the route
of OPCPA pumped by a Yb:YAG thin-disk laser. The first thing is to seek suitable nonlinear
crystals that can highly transmit both near-IR pump and mid-IR signal and more importantly can
support the necessary PM condition for generating tunable sub-picosecond mid-IR pulses.
After a survey, we intend to adopt the non-oxide BGSe crystals [25–27]. The commonly-used
oxide crystals, e.g., β-BBO, LiNbO3 and KTiOAsO4 crystals, are excluded due to the limited
transmission for the mid-IR pulse. Within the non-oxide crystals, the LiGaS2 and BGSe crystals
are picked out because both of them have a high transmission on the 1030-nm pump laser.
Compared to the LiGaS2 crystal, the BGSe crystal has a wider transparent range in the infrared
region [up to 16 µm, black curve in Fig. 2(a)], a larger effective nonlinear coefficient (∼25
pm/V), and a higher damage threshold (∼20 GW/cm2 at 4-ps 1030-nm pump). The BGSe
crystals have been utilized to generate mid-IR pulse via optical parametric oscillation [28],
DFG [29] and optical parametric amplification [30,31]. To judge whether the BGSe crystal is
appropriate to build the sub-picosecond mid-IR OPCPA, we then analyze its PM characteristic at
1030-nm pump. Different from previous designs for broadband OPCPA, here the group-velocity
matching between the signal and idler should be avoided to limit the bandwidth to a value that
corresponds to a sub-picosecond FTL pulse duration. Figure 2(a) plots the group velocity of an
extraordinary-polarized light along the x principal axis of BGSe crystal. The figure suggests
that the strict group-velocity matching may be satisfied around 15 µm in the collinear PM
configuration. In the mid-IR region between 3 to 8 µm that we concern about, the group-velocity
matching is not fulfilled, which is just what we want.
We then calculate the gain wavelengths at different PM angles θ for a 5-mm-thick BGSe crystal.
Only Type-I [e(s)+e(i)→o(p)] collinear PM configuration in the XZ plane of BGSe crystal is
studied due to the maximized effective nonlinear coefficient. The calculated results are given
 Research Article Vol. 31, No. 22 / 23 Oct 2023 / Optics Express 36414

Fig. 2. Phase-matching (PM) characteristics of BGSe crystal. (a) Measured transmission

spectrum of a 5-mm-thick un-coated BGSe crystal (black curve) and calculated group
velocity for the extraordinary-polarized light along the principal axis x of BGSe crystal
(blue curve). (b) Calculated mid-IR spectra versus PM angle for Type-I optical parametric
amplification with a 1030-nm pump and a 5-mm-thick BGSe crystal. The color bar indicates
the normalized small-signal gain.

in Fig. 2(b). Clearly, BGSe supports PM in its entire infrared transparent range, suggesting a
superior spectral tunning ability. As expected, the PM bandwidth is maximized around 15.4 µm
due to the meet of group velocity matching, but becomes narrower in the range of 3 to 8 µm. At
θ = 56°, for example, the bandwidth is confined to ∼ 1 µm with a central wavelength of 4 µm,
corresponding to a FTL pulse duration of 220 fs. Considering the practical gain narrowing effect,
it is feasible to develop sub-picosecond OPCPA based on BGSe crystals.
We design a three-stage OPCPA system based on three BGSe crystals and a Yb:YAG thin-disk
pump laser. The system setup is schematically plotted in Fig. 3. The mid-IR seed pulses for the
OPCPA are generated from a La3 Ga5.5 Nb0.5 O14 (LGN)-based intrapulse DFG setup pumped
by an 800-nm few-cycle laser (Venteon OPCPA, Laser Quantum) [32]. To facilitate spectral
tuning of OPCPA, the LGN rather than BGSe is adopted in the intrapulse DFG because LGN
can generate broader mid-IR spectra than BGSe. The 800-nm laser also provides a seed to the
Yb:YAG thin-disk laser (VaryDsik, Dausinger Giesen GmbH), so the two lasers are optically
synchronized. The pump laser outputs 4-ps pulses at 1030 nm with a 1-kHz repetition rate. To
match the pump pulse duration, the mid-IR seed pulse is stretched to ∼ 4 ps by a 120-mm-long
silicon with 2-6 µm anti-reflection coatings. Three uncoated BGSe crystals with the thickness
of 5, 3.5 and 3 mm, all cut at θ = 55.6° and φ = 0° for Type-I PM, are used in the three OPCPA
stages, respectively. The mid-IR seed beam transmits through the three OPCPA stages freely
without any beam telescopes, ensuring a good mid-IR beam quality. The pump energies for the
three stages are 3.2, 5.5 and 7 mJ, respectively, but with the same pump intensity of ∼10 GW/cm2
through appreciate beam telescopes. The beam spots of both pump and mid-IR signal are smaller
than the crystal aperture in each stage for facilitating angular tunning. After the third OPCPA,
the amplified mid-IR pulse is compressed by a coated 32.5-mm-thick Al2 O3 plate, which is then
sent into the diagnostic optics.
 Research Article Vol. 31, No. 22 / 23 Oct 2023 / Optics Express 36415

Fig. 3. Schematic setup of the sub-picosecond tunable mid-IR OPCPA source. In each
OPCPA stage, a small noncollinear angle between the pump and mid-IR signal is used to
facilitate beam splitting. HWP: half-wave plate; OAP: off-axis parabola mirror with an
effective focal length of 152.4 mm; Ge: a coated germanium filter; Si, a silicon rod as the
stretcher. Al2 O3 , aluminium oxide as the compressor.

4. Results and discussion

Initially, the seed spectrum from the intrapulse DFG is tuned to a range from 3 to 4.5 µm (left
shaded area in Fig. 5) with an effective seed energy ∼2 nJ to subsequent OPCPA. All the BGSe
crystals in three OPCPA stages are preset to a strict PM wavelength of 3.95 µm. The first OPCPA
stage amplifies the mid-IR seed to ∼10 µJ, with a high energy gain of 5000. As shown by the
purple curve in Fig. 4(a), only a small part of the seed spectrum, from 3.9 to 4 µm, is amplified by
the first OPCPA stage, demonstrating a limited gain bandwidth of the BGSe crystal. Considering
the bandwidth effect, the energy gain greatly exceeds 5000 for the amplified spectral components.
After the second OPCPA stage, the mid-IR pulse is boosted to ∼110 µJ and its spectrum shrinks
due to the gain narrowing effect [green curve in Fig. 4(a)]. The mid-IR spectrum further shrinks
after the third OPCPA stage [orange curve in Fig. 4(a)], and the amplified pulse energy reaches
270 µJ at full 7-mJ pump with a pump-to-signal conversion efficiency of 2.4%. To ascertain
the amplified state of the third OPCPA stage, we record the efficiency versus the pump energy
in this stage [Fig. 4(b)]. With the increase of pump energy, the efficiency of the third OPCPA
stage climbs to 2.5% at ∼ 4-mJ pump, then reaches the maximum of ∼2.6% at 5.8-mJ pump,
and finally degrades slightly at the full 7-mJ pump. This demonstrates that the third OPCPA
stage works in deep saturation. The output energy fluctuation is measured to be 1.6% (root mean
square) over ten minutes [Fig. 4(c)]. The peak efficiency can be enhanced by increasing the chirp
of mid-IR seed beam. As shown in the inset of Fig. 4(c), the amplified mid-IR pulse has a good
beam profile, measured by a beam profiler (WinCamDIR-BB, DataRay).
The amplified mid-IR pulse is compressed by a 32.5-mm-thick Al2 O3 rod with anti-reflection
coating, which can well compensate for the second-order dispersion induced by the upstream
transmission elements, e.g., the silicon stretcher and three BGSe crystals. After the compressor,
the pulse energy is ∼260 µJ, with a compression efficiency of 96%. The compressed pulse
duration is detected by an autocorrelator (PulseCheck USB MIR, APE). As given in Fig. 4(d),
the measured pulse duration is ∼590 fs (FWHM) assuming a deconvolution factor of 1.543 for
hyperbolic secant profile. Such a pulse duration is very close to the optimal FTL pulse duration
required by the high-efficiency OR, as given in Section 2. The difference between the measured
 Research Article Vol. 31, No. 22 / 23 Oct 2023 / Optics Express 36416

pulse duration here and the expected value of 220 fs in Section 2 is caused by the gain narrowing
effect in the three-stage OPCPA, as shown in Fig. 4(a).
As an all-parametric system, the mid-IR light source has good spectral tuning ability, as shown
in Fig. 5. The LGN-based intrapulse DFG can provide broadband mid-IR seed, tunable in the
range of 3 to 7 µm [32]; and here two separate spectral packets with an overlap (shaded areas
in Fig. 5) are used to seed the OPCPA system, alternatively. Thanks to the PM capability of
the BGSe crystal [Fig. 2(b)], the output wavelength of the sub-picosecond light source can be
continuously tuned within the seed spectral range (i.e., 3 to 7 µm) via steering the crystal angles.
In our experiments, the long-wave edge of the spectral tunability is only measured up to 5 µm,
which is limited by the spectral response of our spectrometer (Mozza, Fastlite). The eight spectra
given in Fig. 5 have similar profiles with limited bandwidths, all corresponding to sub-picosecond
FTL pulses. The pulse energies are also monitored when tuning the spectra, all of which exceed
200 µJ before compression (red squares in Fig. 5). The difference on the output energies of the

Fig. 4. Output performance of the three-stage OPCPA system centered at 3.95 µm. (a)
Mid-IR spectra after different OPCPA stages. (b) Pump-to-signal conversion efficiency
versus the pump energy for the third OPCPA stage. (c) Amplified mid-IR pulse energy
within 10 minutes (black curve) at the highest efficiency point in Fig. 4(b) and the mid-IR
beam profile (inset). (d) Measured autocorrelation trace of the output pulses after the third
OPCPA stage (black dots) and its Gaussian fit (red curve).
 Research Article Vol. 31, No. 22 / 23 Oct 2023 / Optics Express 36417

Fig. 5. Spectral tunability of the mid-IR source. Solid curves show the amplified spectra
after the third OPCPA stage via angular tuning. Red squares mark the corresponding pulse
energy for each spectrum. With the angular tuning, the time delay between the pump and
seed is optimized to maximize the output energy. Two grey areas indicate the seed spectra
after the intra-pulse DFG at two different PM angles.

eight spectra is mainly caused by different seed energies. Higher mid-IR output is expected by
using larger-size BGSe crystals as well as higher pump energy.
Above, we demonstrate a mid-IR OPCPA source based on BGSe crystals. It can generate
millijoule-class sub-picosecond mid-IR pulses tunable in the range from 3.5 to 5 µm or beyond.
Such a mid-IR light source is tailored for pumping OR. Both the mid-IR wavelength and
sub-picosecond pulse duration are helpful to enhance the pump-to-THz conversion efficiency, as
shown in Section 2. In principle, the achievable spectral range of this light source extends well
beyond the infrared transparence edge of the LiNbO3 material. Therefore, this light source can
also be used to pump OR in other materials, such as ZnTe [33], GaAs [34], ZnGeP2 [35] and
BGSe [36].

5. Conclusion
In summary, we have developed a tunable mid-IR light source with a sub-picosecond pulse
duration, which is tailored for driving high-efficiency optical rectification. The system consists
of an LGN-based intrapulse DFG stage and three BGSe-based OPCPA stages, pumped by a few-
cycle 800-nm laser and a Yb:YAG thin-disk laser, respectively, with all-optical synchronization.
The output pulses can be tuned in the range of 3.5 to 5 µm with a good beam profile. The
sub-picosecond FTL pulse duration is contributed by the phase-matching characteristic of BGSe
crystals. To the best of our knowledge, it is the first OPCPA experiment with BGSe crystals, and
it is also the first light source specifically developed for optical rectification. Such a light source
offers more degrees of freedom to enhance the laser-to-THz efficiency for the optical rectification
in various materials.
Funding. National Natural Science Foundation of China (62375165, 62122049, 91850203, 61975120); Science and
Technology Commission of Shanghai Municipality (21QA1404600, 22JC1401900).
Acknowledgments. We thank the support from the Fundamental Research Funds for the Central Universities. J.
Ma would like to thank the sponsorship of the Yangyang Development Fund and the Cyrus Tang Foundation through the
Tang Scholar program.
Disclosures. The authors declare that there is no conflict of interest regarding the publication of this article.
Data Availability. Data underlying the results presented in this paper are not publicly available at this time but may
be obtained from the authors upon reasonable request.
 Research Article Vol. 31, No. 22 / 23 Oct 2023 / Optics Express 36418

Supplemental document. See Supplement 1 for supporting content.

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