Le et al.

Light: Science & Applications (2023)12:34 Official journal of the CIOMP 2047-7538
https://doi.org/10.1038/s41377-023-01071-z www.nature.com/lsa

ARTICLE Open Access

A novel scheme for ultrashort terahertz pulse

generation over a gapless wide spectral range:
Raman-resonance-enhanced four-wave mixing
1,3 ✉
Jiaming Le1, Yudan Su2, Chuanshan Tian , A. H. Kung1 and Y. Ron Shen1,2 ✉

Abstract
Ultrashort energetic terahertz (THz) pulses have created an exciting new area of research on light interactions with
matter. For material studies in small laboratories, widely tunable femtosecond THz pulses with peak field strength close
to MV cm−1 are desired. Currently, they can be largely acquired by optical rectification and difference frequency
generation in crystals without inversion symmetry. We describe in this paper a novel scheme of THz pulse generation
with no frequency tuning gap based on Raman-resonance-enhanced four-wave mixing in centrosymmetric media,
particularly diamond. We show that we could generate highly stable, few-cycle pulses with near-Gaussian spatial and
temporal profiles and carrier frequency tunable from 5 to >20 THz. They had a stable and controllable carrier-envelop
phase and carried ~15 nJ energy per pulse at 10 THz (with a peak field strength of ~1 MV cm−1 at focus) from a
0.5-mm-thick diamond. The measured THz pulse characteristics agreed well with theoretical predictions. Other merits
of the scheme are discussed, including the possibility of improving the THz output energy to a much higher level.
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Introduction essentially the whole spectral range from ~10 THz to soft
The advent of intense ultrashort coherent light pulses has X-ray even in ordinary laboratories. Below ~5 THz, high-
revolutionized the spectroscopy field1–3. On one hand, they intensity picosecond pulses exist7, but between 5 and
allow easy observation of various nonlinear optical effects 12 THz, stable, continuously tunable, energetic fs pulses
and facilitate characterization of materials with nonlinear are more difficult to come by8–10. Yet this is a spectral
optical spectroscopy. On the other hand, they provide range of great importance for materials studies. Phonons
means for strong selective excitation of materials, and and vibrations of molecules and solids composed of heavier
optical manipulation of material structure and properties atoms are in this range, and so are the intermolecular (or
such as optical-field-induced ferroelectricity, super- inter-molecular-group) vibrations of molecular systems in
conductivity, and others4–6. They have also created the chemistry and biology. Various elementary excitations of
vibrant field of ultrafast dynamics of low-frequency exci- solids also lie in this spectral region. In the review article on
tations in materials1. Thanks to advances in laser tech- “The 2017 Terahertz Science and Technology Roadmap”,
nology over the past decades, intense femtosecond (fs) the 5 to 15 THz spectral range was labeled as the present-
pulses from table-top setups are now available over day THz gap calling to be filled8,9.
Currently, optical rectification (OR) or difference fre-
quency generation (DFG) in second-order nonlinear crys-
Correspondence: Chuanshan Tian (cstian@fudan.edu.cn) or
tals is the common technique to generate intense THz
Y. Ron Shen (yrshen@berkeley.edu)
1
Department of Physics, State Key Laboratory of Surface Physics and Key pulses. However, because of phonon absorption, THz
Laboratory of Micro- and Nano-Photonic Structure (MOE), Fudan University, generation from crystals is limited. For example, GaSe is
Shanghai 200433, China
2 among the few best nonlinear crystals for THz genera-
Department of Physics, University of California, Berkeley, CA 94720, USA
Full list of author information is available at the end of the article tion11–13, but it has several absorption bands between
These authors contributed equally: Jiaming Le, Yudan Su

© The Author(s) 2023

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction
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Le et al. Light: Science & Applications (2023)12:34 Page 2 of 7

10 and 20 THz and a precipitous drop in transmission achievable in wide band gap materials with two of the
below 10 THz14,15. The strong dispersion of the reststrahlen inputs exciting a Raman resonance. Of these materials,
band at ~8 THz limits the effective coherent length of fs diamond is most attractive because of its unique absorp-
DFG in GaSe to ~200 μm in the 10–20 THz range (with tion spectrum (see Supplementary Information, SI, for
pump wavelength around 1 µm) and distorts the THz more details).
temporal profile. The effective coherence length becomes Diamond has no intrinsic absorption throughout the
much less than 100 μm below 10 THz. Organic nonlinear spectral range from 0 to 5.5 eV (44,000 cm−1) except for
crystals have been used for efficient THz generation, but some minor absorption between 1600 and 4000 cm−1 due
they have only a few narrow transparent windows above to multi-phonon transitions. It possesses a nonresonant
5 THz and suffer from low optical damage thresholds16. χ(3) of ~4.6 × 10−14 esu (6.4 × 10−22 m2 V−2) that is reso-
Laser-induced gas plasmas can generate energetic THz nantly enhanced to ~6 × 10−12 esu (8 × 10−20 m2 V−2)
pulses with spectra peaked at low THz and a broad wing near the Raman resonance at 40 THz24. The optical
extending to >50 THz. They are well suited as probes for damage threshold of a typical CVD diamond plate is
linear THz spectroscopy over a wide spectral range, but ~7 TW cm−2 for ~60 fs pulses at 50 THz in the infrared
their complex spatial mode patterns make them less desired (measured value on our CVD diamond at 50 THz). With
as pumps for strong resonant excitations17–19. Free electron all three inputs in the infrared, noncollinear phase
lasers and electron-driven THz sources can also produce fs matching in four-wave mixing is possible from 2.5 to
pulses covering the entire THz spectral range20,21, but they >100 THz. We report here a successful demonstration of
are not readily available for most researchers. One may THz generation by resonant four-wave mixing (R-FWM)
think four-wave mixing as a frequency conversion process in diamond. We were able to generate stable, few-cycle,
could generate desirable THz pulses from materials if the transform-limited THz pulses that were tunable from 5 to
input beams are sufficiently intense. >20 THz with controllable carrier-envelope phase (CEP)
Indeed, THz generations by four-wave mixing22 and and had ≥10 nJ per pulse. This THz generator nicely
seeded optical Kerr amplification23 in crystals were pro- covers the existing THz gap in THz spectroscopy8,9. We
posed earlier, but they ran into difficulties in practice. The summarize in Table 1 the data on THz pulse generation
third-order nonlinear susceptibilities of materials are by different schemes commonly used in small laboratories
small (χ(3) ~ 10−14 to 10−15 esu or 10−22 to 10−23 m2 V−2). for comparison.
Generation of >10 nJ THz pulses requires input pulses
with peak intensities higher than a few TW cm−2, which is Theory for THz generation by Raman-resonant four-wave
above the optical damage threshold of most materials. mixing in diamond
The scheme can be made practical only if χ(3) of a material The basic theory behind resonant four-wave mixing
can be greatly enhanced through resonances while the (R-FWM) is straightforward. The three pulsed inputs,
optical damage threshold is still sufficiently high. This is described by ~ r; t Þ ¼ ~
Ei ðωi ;~ r; t Þ expði~
Ei ð~ ki ~
r  iωi tÞ with

Table 1 Summary of THz generation schemes commonly used in small laboratories

Scheme Reference Input parameters Output characteristics

Wave-length Pulse energy Peak freq. (THz) Bandwidth (THz) Pulse energy Conversion (‰)
(μm) (μJ) (μJ)

25
OR in LiNbO3 Ref. 0.8 6.5 × 103 0.35 0.5 6.4 1
26 a
Gas plasma Ref. 0.8 560 6 12 ~0.06 ~0.1a
11
DFG in GaSe Ref. 1.1 ~300 30 10 1.7 ~6
~1.2 ~300
DFG in GaSe Ref. 13
1.03 ~3 13 6 1.5 × 10–3, b
0.5b
1.07 4.7
R-FWM in This work 1.45 85 5 9 5 × 10–3 0.5
diamond 1.80 35 10 1.5 × 10 –2
1.5
–2
~6 10 15 4.1 × 10 4
a –4
Estimated with 10 yield
b 13
Scaled from THz generation at higher frequency in ref. . The pulse repetition rate was 190 kHz
Le et al. Light: Science & Applications (2023)12:34 Page 3 of 7

a b
1.0
1 S
1 2 Q 0.8

Q (t ) (a.u.)
0.6
2 3 250 ps
S 3
r
50 ps
0.4
r
10 ps
k1 4 ps
R ks 0.2 1.3 ps
θ 0.1 ps
Q r r 0.0
g k2 k3 –20 –10 0 10 20 30
Time (ps)

c d 12 THz 10 THz 8 THz 6 THz

1.0
θ 0.42° 11 THz 9 THz 7 THz 5 THz
Spectral density (a.u.)

0.8 0.51°
0.59°
0.65°
0.6
0.71°
0.4

0.2

0.0
5 10 15 20 25
Frequency (THz)
0 2 4 6 8 10 12 14 16 mm

Fig. 1 THz generation by R-FWM in diamond. a Energy level diagram, Feynman diagram, and wave-vector diagram describing four-wave mixing
with a Raman resonance. b Time variation of the 1332 cm−1 vibrational wave in diamond coherently excited by ~ E1 and ~
E2 pulses of different pulse
widths. c Calculated THz output spectra at selected θ. d Calculated spatial distributions of different frequency components in the collimated THz
output beam for the case of θ = 0.42° in c; each circle describes a Gaussian distribution cut off at e−2 of the maximum

center frequency ωi (i = 1, 2, and 3), induce a third-order Fig. 1b is the calculated Q(t) for diamond under Gaussian
nonlinear polarization ~ P ð3Þ ðωS ¼ ω3  ω1 þ ω2 ;~ r; t Þ with pulse excitation of ~ E1 ðt Þ~
E2 ðt Þ with different pulse widths. It
center frequency at ωS in a medium, where ω1  ω2  ωR is seen that for a pulse width of 1.3 ps, Q(t) can reach a peak
with ωR being the Raman resonance frequency (Fig. 1a). value of ~30% of
Qst in diamond with a corresponding
Knowing ~ P ð3Þ ðωS ;~r; t Þ, we can solve the wave equation to χ⃡ 3res ðt Þ  0:3 χ⃡ 3res st .
find the output field ~ ES ðωS ;~ r; t Þ. For generation of fs THz With ~ r; t Þ known from given ~
P ð3Þ ðωS ;~ r; t Þ; ~
E1 ð~ E2 ð~
r; t Þ and
pulses, however, a few details should be noted (see SI for ~E3 ð~ r; t Þ, we can find the THz output by solving the wave
details). The Raman linewidth of diamond is ~1.25 cm−1, equation or by numerically calculating the output field from
corresponding to a ~4 ps vibrational dephasing time. This the dipole radiation equation28. Details of the calculations
means that fs input pulses of ~ E1 and ~ E2 can only excite the are presented in SI. For quantitative evaluation, we con-
Raman resonance weakly. To fully benefit from the sidered the case of 1.3 ps E1 and E2 pulses at 206 and
Raman resonance enhancement of χ(3), we must employ 166 THz, respectively, to excite the Raman resonance of a
picosecond ~ E1 and ~ E2 pulses for excitation. 500-μm diamond (001) plate and a 60 fs E3 pulse with center
The R-FWM process can be understood as follows27: The frequency tunable from 45 to 60 THz to generate 5 to
ps ~E1 and ~ E2 input pulses coherently excite the transient 20 THz output; all beams were p-polarized along [110] and
vibrational wave, Q ~ð~ r; t Þ, associated with the Raman reso- incident on diamond at ~45°. The wave vector diagram
nance in diamond; the fs ~ E3 input pulse then beats with the sketched in Fig. 1a shows that noncollinear phase matching
vibrational wave in diamond at a selected time to create the of the R-FWM process is possible. For each θ between ~ k1
fs THz pulse. We can find Q ~ð~ r; t Þ from given ~ E1 ð~
r; t Þ and and ~ k2 ||~k3 , there is a corresponding phase-matched (PM)
~
E2 ð~
r; t Þ by solving the equation of motion for Q ~ð~ r; t Þ. We THz output with a bandwidth of a few THz that satisfies the
can write Qðt Þ  f ðt ÞQst , where Qst / E1m E2m is the near-phase-matching condition of Δkl=2 < 1, where l is the
steady-state Q(t) that would appear if E1 ðt Þ and E2 ðt Þ with beam path length in diamond24. Thus, the transform-limited
peak values of E1m and E2m were long pulses. Beating of THz output should appear as fs pulses. The calculated THz
~
E3 ð~
r; t Þ and Q ~ð~ r; t Þ then induces ~ r; t Þ ¼ χ⃡ ð3Þ
Pð3Þ ðωS ;~ res ðt Þ : output spectra for different θ are described in Fig. 1c.
~  ~~
E1m ðr ÞE2m ð~ ~
r ÞE3 ð~ ð3Þ ð3Þ
r; t Þ with χ⃡ res ðtÞ ¼ f ðtÞðχ⃡ res Þst . Plotted in Because of the ω2S dependence of THz generation, the peaks
Le et al. Light: Science & Applications (2023)12:34 Page 4 of 7

of the spectra are blue shifted from those expected from PM. Experimental arrangement
The near-PM requirement also leads to emission of different In the experiment, we used a commercial 33-fs,
THz components in different directions with different 5-W,1-kHz Ti:sapphire laser system to pump two optical
angular spreads (see SI and Fig. S3). Collimation after the parametric amplifiers (OPA) seeded by a common white
beam exit from diamond makes different THz components light source. (Details of the experimental arrangement is
appear with differently displaced near-circular Gaussian given in SI). The signal and idler from OPA-1 centered at
distributions in the collimated beam. Figure 1d is an example ω1/2π = 206 THz and ω2/2π = 166 THz were stretched to
showing the PM 5 THz distribution at the center and those 1.3-ps positively chirped pulses with a constant instanta-
of other frequency components away from the center. neous difference frequency of 40 THz. The ω3 pulses of 63-
Focusing of the collimated beam or imaging of the beam exit fs width, tunable between 40 and 60 THz were derived from
from diamond recombined all the THz frequency compo- OPA-2 with a difference frequency generation stage. All
nents at the image position. three p-polarized pulses were incident on a 0.5-mm (001)-
For a crude estimate on the THz output, we can use the cut diamond plate at ~45° and overlapped over an area
usual expression for output energy per pulse from wave inside diamond of π(140 × 100)/2 μm2. The p-polarized
mixing under the pump-depletion-less limit. The energy THz outputs were characterized by knife-edge beam pro-
per pulse for THz generation from phase-matched four filing, a Fourier transform infrared interferometer (FTIR)
wave mixing is given by: and electro-optic sampling (EOS) (see SI for details).
16π 4 ω2S 2 W ðω1 ÞW ðω2 Þ
W ðωS Þ  χ ð3Þ l W ðω3 Þ Results
c4 nn n
1 2 3 S n A2 T 2 Figure 2a shows a set of measured THz spectra gener-
in cgs units, where A is the beam overlapping area, T is the ated by R-FWM with the beam geometry set to have θ at
pulse width of ~ E1 and ~ E2 , and l is the interacting path 0.42°, 0.51°, 0.59°, 0.65°, and 0.71°. The input energies per
ð3Þ
length. For the diamond case, if we take jχ ð3Þ j ¼ 0:3jðχ res Þst j pulse were W1 ≈ 85 μJ, W2 ≈ 35 μJ and W3 ≈ 10 μJ on the
12 −20 2 −2
 2 ´ 10 esu (~3 × 10 m V ), l = 0.5 mm, W(ω1) = overlapping area. The corresponding spectra of the ω3
W(ω2) = 40 μJ, W(ω3) = 10 μJ, A = 4 × 10−4 cm2, and input pulses generating the THz spectra are given in
T = 1.3 ps, we find W(ωs) ~ 14 nJ per pulse at ωs/ Fig. 2b. It is seen that the two sets of spectra are very
2π = 10 THz with a pulse width nearly the same as that similar as expected except for an overall shift of 40 THz
of the ~
E3 input. This suggests that R-FWM in diamond can and some deviation due to the ω2S dependence of THz
be a powerful THz generator. generation. The measured THz spectra can be well fit by

a b c
40
THz energy (nJ)

THz spectra E 3 pulse spectra Measured

Expt. 30 Calculated
Theory
Normalized spectral intensity (a.u.)

Normalized spectral intensity (a.u.)

20
10
0
5.0 7.5 10.0 12.5 15.0 17.5
(3–R) / 2 (THz)
W3 (μJ)
d 0 2 4 6 8 10
THz energy (nJ)

40 40
30 30
20 20
10 10
5 10 15 20 25 40 45 50 55 60 65 0 0
0 2 4 6 8 10
Frequency (THz) Frequency (THz)
W1W2 (103 μJ2)

Fig. 2 Experimental results on R-FWM in diamond. a THz output spectra: top to bottom frames for beam geometry set to have the THz frequency
PM at 5, 7.5, 10, 12.5, and 17 THz, respectively. Solid curves are theoretical fits. b Measured one-to-one corresponding spectra of the converting ~E3
pulses with respect to the THz spectra in (a). c Output THz energy per pulse (circles) for the five beam geometries set in a and calculated THz energy
(curve) using χ ð3Þ ¼ 2:8 ´ 1012 esu. d Data showing the linear dependences of THz pulse energy on energy product of ω1 and ω2 pulses and on
energy of the ω3 pulse
Le et al. Light: Science & Applications (2023)12:34 Page 5 of 7

a c e 1
1
6 0
π
THz Energy (nJ)

E THz (a.u.)
E THz (a.u.)
4
0 0

–1 –1
0
–20 –10 0 10 20 –0.8 –0.4 0.0 0.4 0.8 –0.4 –0.2 0.0 0.2 0.4
Detuning (cm–1) Time (ps) Time (ps)

b 6 d 90
f THz energy (a.u.)
1.0 90°
120° 60°
THz energy (nJ)

Expt.
Amplitude (a.u.) 45

Phase (deg)
4 Fitting 150° 30°
0
0.5
2 180° 0°
–45

0 –90 210° 330°

0.0
0 5 10 15 4 6 8 240° 300°
Delay (E 3, Q) (ps) Frequency (THz) 270°

Fig. 3 Characteristics of THz generation by R-FWM in diamond. a THz output energy versus resonance detuning. b Dependence of THz output
energy with time relative to the vibration excitation Q(t) and its fit with |Q(t)|2. c Temporal trace of a THz pulse with PM at 5 THz measured by EOS in
GaP. d Amplitude and phase spectra from Fourier transform of the THz pulse in (c). e THz pulses with CEP of 0 (red curve) and π (blue curve).
f Measurement (scatters) and fitting (solid curve) of polarization distribution of 17 THz output showing that the THz pulses were linearly polarized

theory as described in Fig. 2a. The total THz energy We also characterized the THz output in the time
versus the THz frequency ω3  ωR is plotted in Fig. 2c. It domain by EOS. The result for a THz output pulse PM at
is 5 nJ per pulse at 5 THz and increases to 41 nJ per pulse 5 THz is displayed in Fig. 3c with its Fourier-transformed
at 17 THz. In Fig. 2d, the output energy, W(ωs), is seen to amplitude and phase spectra in Fig. 3d. Due to absorption
be linearly proportional to the input energies, W1W2 and at higher THz frequencies in the EOS crystal, the EOS
W3, as it should be. From the measured THz energies, temporal trace was distorted into a broader pulse and a
ð3Þ
we were able to deduce jðχ res Þst j  9 ´ 1012 esu corresponding narrower FT spectrum compared to that
−19 2 −2
(~1 × 10 m V ), compared to 6 ´ 1012 esu in ref. 24 measured directly by FTIR. The observed uniform spectra
We also used a slit of variable width placed at various phase in Fig. 3d however implies that the THz pulse
positions in the output beam to map out the spatial dis- should be nearly transform-limited with a pulse width of
tribution of the THz output spectrum and found good ~70 fs. If such a pulse is focused to an area of ~(100 μm)2,
agreement with theoretical prediction (see SI and Fig. S6). the peak electric field of 10 and 17 THz pulses with energy
As expected, the THz output was spatially chirped (see of 15 nJ and 41 nJ can reach about 1 and 1.7 MV cm−1,
Fig. 1d). With a pair of parabolic mirrors, the THz output respectively. The THz pulses were CEP locked, and the
re-focused at the image point appeared as transformed- phase could be controllably changed by varying the time
limited fs pulses (see SI and Fig. S7). An appropriate delay of the ω3 pulse (see SI). Figure 3e shows two mea-
aperture in the THz beam path could select a specific sured THz pulses with CEP adjusted to 0 and π; a time
portion of the THz output to yield a THz pulse with the delay of 13 fs of the ω3 pulse led to a CEP change of π. The
desired spectral and temporal profiles. THz output generated was linearly polarized in the same
Figure 3a provides a description on the effect of plane as the inputs as described in Fig. 3f.
detuning of excitation from Raman resonance. As ω1 
ω2 moves away from the resonance, the observed THz Discussion
output drops as predicted. In another measurement, the The above results constitute the first demonstration
overlapping time of the fs E3 pulse with the excited that R-FWM in centrosymmetric condensed media can
vibration, Q(t), was varied, the THz output went be effective to generate energetic THz pulses. Diamond,
through a peak and then decayed, mapping out the in particular, has attractive merits. Its high optical
variation of Q(t), as depicted in Fig. 3b. Theoretical fit of damage threshold allows input pump intensities to be so
the data allowed the deduction of the phonon dephasing high as to induce third-order nonlinear optical effects
time, T2 = 4.8 ps. (e.g., FWM) competing with second-order effects
Le et al. Light: Science & Applications (2023)12:34 Page 6 of 7

(e.g., DFG) in other crystals. Transparency throughout duplicating the characteristics of the input pulse except
the region from THz to UV leads to weak frequency for the frequency shift. An input pulse of high quality, in
dispersion of optical response coefficients that facilitates terms of spatial, spectral, and temporal profiles as well as
phase-matched THz pulse generation over a very wide amplitude and phase stability, generates a THz pulse of
spectral range with exceptionally good quality. With the nearly equal high quality. Tuning the characteristics of the
phonon mode Raman-excited by ps pulses, the coherent input pulse tunes the characteristics of the THz output
phonon wave hardly changes on the fs time scale. It is pulse accordingly. In this respect, we can amplitude- or
then seen that R-FWM for fs THz pulse generation in polarization-modulate the THz pulse simply by mod-
diamond is effectively a beating process between a fs IR ulating the input pulse29.
pulse with a constant phonon wave or a frequency con- With a fs commercial laser system, we were able to use
version process down-converting the fs IR pulse by the R-FWM in diamond to generate stable fs THz pulses over
phonon wave to the fs THz pulse. The latter essentially a wide spectral range with very high quality. The THz
duplicates the input fs IR pulse except for a shift in fre- output energy was >10 nJ (producing a peak field strength
quency and some modification due to radiation effi- ~1 MV cm−1 at a 100-μm focal spot) at 10 THz, and
ciency. Thus, the characteristics of the THz pulse can be higher for higher THz frequencies. It could be enhanced
readily tuned by tuning the corresponding characteristics by at least one order of magnitude with a higher input
of the input IR pulse. The energy conversion efficiency is pulse energy and a thicker diamond plate. We also note
given directly by the ratio of the output THz pulse energy that R-FWM in diamond can be collinearly phase-
to the input fs pulse energy. We have measured phase- matched if the diamond plate is made birefringent by
matched THz pulse generation with the center frequency uniaxial stress of ~1 GPa. Growth of CVD diamond to
spanning from 5 to 20 THz, but this spectral range can be >6 mm thick was recently reported30; collinear PM in
readily extended to >100 THz. As the THz radiation such a diamond plate would push R-FWM toward the
efficiency increases with square of the frequency, and pump depletion region and a THz output of >1 μJ per
there is more pulse energy at higher input frequency, we pulse should be easily attainable with an input of ~10 μJ
expect the output energy at higher THz frequency gen- per pulse from the converting pulses, corresponding to a
erated by R-FWM in diamond can reach a level com- peak THz field strength of a 50 fs THz pulse to
parable to that generated by DFG in GaSe or other >10 MV cm−1 if focused to an area of ~(100 μm)2.
crystalline compounds.
As a first demonstration of THz generation by R- Acknowledgements
Our thanks are due to Ya Cheng (East China Normal University) for his help on
FWM, we have not optimized the parameters in our pulse stretcher, Chih-Hsuan Lu and Jhan-Yo Guo (Tsing Hua University) for
experiment. We can increase the peak intensities of the their assistance on the experimental setup, and Chao-Nan Lin and Chong-Xin
three input pulses on diamond by an overall factor of 10 Shan (Zhengzhou University) for providing CVD diamond plates. This work was
supported by the National Natural Science Foundation of China Grants (No.
before reaching the optical damage threshold. Doubling 12125403 and No. 11874123) and the National Key Research and Development
the diamond thickness would increase the conversion Program of China (No. 2021YFA1400503 and No. 2021YFA1400202).
efficiency by ~4. If more input energy from the laser
system is available to pump a larger area of diamond, Author details
1
Department of Physics, State Key Laboratory of Surface Physics and Key
the THz output energy can be further improved in Laboratory of Micro- and Nano-Photonic Structure (MOE), Fudan University,
proportional to the beam area. While the R-FWM Shanghai 200433, China. 2Department of Physics, University of California,
scheme is more complex in experimental arrangement, Berkeley, CA 94720, USA. 3Collaborative Innovation Center of Advanced
Microstructures, Nanjing 210093, China
it has obvious merits compared to the other schemes
listed in Table 1, namely, the wide tunability of the Author contributions
center frequency and band width of the fs THz pulses, Y.R.S. conceived the idea. Y.R.S., A.H.K., J.L., and Y.S. designed the experiment.
their near-Gaussian spatial and temporal profiles, and J.L. and Y.S. developed the theoretical framework, performed the calculation,
conducted the experiment, and analyzed the data with guidance from Y.R.S.
the relatively high conversion efficiency from IR input and A.H.K. All authors participated in discussions over research progresses.
to THz output. Y.R.S., Y.S., and J.L. wrote the paper with input from all authors. C.T. supervised
and managed the project, secured funding, and carried general responsibility.
Summary and prospects
Data availability
Our study has unequivocally established that R-FWM in All data are available in the main text or the supplementary materials.
diamond can be made into a high-quality, powerful, fs
THz generator over a wide spectral range without any Conflict of interest
gap. For fs THz pulse generation, R-FWM in diamond can The authors declare no competing interests.
be regarded as a direct frequency down-conversion pro-
cess that converts a fs input pulse at higher frequency Supplementary information The online version contains supplementary
to a fs THz pulse that has characteristics essentially material available at https://doi.org/10.1038/s41377-023-01071-z.
Le et al. Light: Science & Applications (2023)12:34 Page 7 of 7

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