5110 OPTICS LETTERS / Vol. 38, No.

23 / December 1, 2013

Femtosecond-laser pumped CdSiP2 optical

parametric oscillator
producing 100 MHz pulses centered at 6.2 μm
Zhaowei Zhang,1,* Derryck T. Reid,1 S. Chaitanya Kumar,2 Majid Ebrahim-Zadeh,2,3 Peter G. Schunemann,4
Kevin T. Zawilski,4 and Christopher R. Howle5
1
Scottish Universities Physics Alliance (SUPA), Institute of Photonics and Quantum Sciences, School of Engineering and
Physical Sciences, Heriot-Watt University, Edinburgh EH14 4AS, UK
2
ICFO—Institut de Ciencies Fotoniques, Mediterranean Technology Park, 08860 Castelldefels, Barcelona, Spain
3
Institucio Catalana de Recerca i Estudis Avancats (ICREA), Passeig Lluis Companys 23, Barcelona 08010, Spain
4
BAE Systems, MER15-1813, P.O. Box 868, Nashua, New Hampshire 03061, USA
5
Defence Science and Technology Laboratory, Porton Down, Salisbury SP4 0JQ, UK
*Corresponding author: [Link]@[Link]
Received September 2, 2013; revised November 2, 2013; accepted November 2, 2013;
posted November 4, 2013 (Doc. ID 196851); published November 25, 2013
We report the first, to the best of our knowledge, femtosecond-laser-pumped optical parametric oscillator (OPO)
based on the newly developed nonlinear crystal, CdSiP2 . The OPO was synchronously pumped by a mode-locked
Yb:KYW/Yb:fiber master-oscillator power amplifier, providing 1.053 μm pump pulses with durations of 130 fs at a
repetition rate of 100 MHz. The 0.5-mm-thick CdSiP2 crystal was cut for a type-I noncritical interaction, providing a
broad phase-matching bandwidth and ensuring excellent temporal overlap among the pump, signal, and idler
pulses. The OPO generated signal pulses with a spectral coverage over 1260–1310 nm and mid-infrared idler pulses
with a broad spectral coverage at 5.8–6.6 μm (6.2 THz). With a 2% output coupler (OC), the threshold pump power
was 600 mW. At the maximum pump power of 1.6 W, 0.55 W was absorbed due to two-photon absorption and
residual linear absorption in the CdSiP2 crystal, 0.75 W was transmitted, and 53 mW signal power was extracted
through the OC. We estimate that the generated idler power was 24 mW. © 2013 Optical Society of America
OCIS codes: (140.7090) Ultrafast lasers; (190.4410) Nonlinear optics, parametric processes; (190.4970) Parametric
oscillators and amplifiers; (190.7110) Ultrafast nonlinear optics.
[Link]

Yb-based femtosecond-laser sources have shown them- identified type-II and type-III routes to 9.5 μm using
selves to be promising, power-scalable platforms for 1.064 μm pumping, validated by experimental difference
pumping optical parametric oscillators (OPOs) generat- frequency generation (DFG) data at wavelengths up to
ing wavelengths in the mid-infrared (mid-IR) [1,2]. The 9.5 μm [9]. These results, all of which were obtained in
extension of wavelength coverage to beyond 5 μm is low-repetition-rate or Q-switched mode-locked regimes,
made difficult by the lack of nonlinear materials combin- motivated us to investigate the performance of CSP in a
ing transparency at the pump and idler wavelengths cw-mode-locked configuration, promising the possibility
with suitable phase-matching and mechanical properties. of continuous ultrabroadband mid-IR light for Fourier-
Common oxide-based nonlinear crystals (e.g., KTiOPO4 transform and frequency-comb OPO spectroscopy.
and LiNbO3 ) perform well only below 4 μm, with the CSP is transparent from 0.5 to 9 μm, and can be manu-
output power falling off significantly at longer wave- factured with high optical quality and low residual loss. It
lengths due to strong multiphonon absorption. To access has a good thermal conductivity (13.6 W K−1 m−1 ), facili-
the important long-wavelength mid-IR region at more tating high-power operation. The nonlinear coefficient of
than 4 μm, nonoxide crystals, such as AgGaSe2 , CdSe, CSP (d36  84.5 pm V−1 ) is the highest among all nonlin-
ZnGeP2 , or orientation-patterned (OP) GaAs, need to be ear crystals that can be pumped at 1 μm [8]. Indeed, the
employed. Both AgGaSe2 and CdSe are transparent nonlinear figure of merit (defined as d2 ∕n3 , where d is the
from 0.75 to 15 μm, but to avoid two-photon absorption nonlinear coefficient and n is the index of refraction) of
(TPA) during ultrashort pulse operation, they need CSP is ∼300 pm2 V−2 [8], among the best of all known
to be pumped at above 1.5 μm by another OPO [3,4] nonlinear optical crystals. For comparison, the nonlinear
or an Er3
laser, and so are unable to take full advantage figure of merit of PPLN is ∼60 pm2 V−2 . In addition, CSP
of Yb-based pump sources. Similarly, ZnGeP2 and OP is the only nonlinear crystal that can offer noncritical
GaAs-based ultrafast OPOs need to be pumped with phase matching (NCPM) for a 1 μm-pumped OPO with
Tm3
or Ho3
lasers operating above 2.1 μm [5] or an idler output in the 6 μm region.
tandem-pumped by another OPO [6]. The synchronously pumped CSP OPO was based on
In this Letter, we introduce the first example of a the configuration shown in Fig. 1. The pump source
femtosecond-laser-pumped OPO based on the newly (described further in [15]) comprised a 100 MHz semicon-
developed nonlinear crystal, CdSiP2 (CSP), which was ductor saturable absorber mirror (SESAM) mode-locked
recently identified as a promising material allowing Yb:KYW master laser, followed by a Yb-doped fiber
efficient type-I phase-matched nonlinear conversion amplifier, and a pair of transmission gratings for pulse
to >6 μm when pumped at near 1 μm [7–14]. Recent compression. The −3 dB pulse duration was measured
work on the phase-matching properties of CSP has even to be 130 fs, and the spectrum had a central wavelength
0146-9592/13/235110-04$15.00/0 © 2013 Optical Society of America
 December 1, 2013 / Vol. 38, No. 23 / OPTICS LETTERS 5111

Fig. 1. OPO layout. HWP, half-wave plate; M, mirror; L, lens;

OC, output coupler.

at 1053 nm and a −10 dB bandwidth of 27 nm (7.3 THz).

After passing through a Faraday rotator, the maximum
average pump power was 1.7 W. The pump was linearly
polarized, and the polarization direction could be con-
trolled by a half-wave plate.
The CSP crystal was cut at θ  90°, φ  45° for type-I
(e → o
o) NCPM and had a thickness of 0.5 mm. Its Fig. 2. Noncritical (θ  90°) type-I (e → o
o phase-match-
aperture was 4 mm × 5 mm. Both crystal surfaces were ing efficiency maps for a 0.5-mm-thick CSP crystal at pump
antireflection (AR) coated with a single-layer sapphire wavelengths from 1040 to 1070 nm.
coating (TwinStar Optics), providing high transmission
(>99%) for the pump and signal from 1035 to 1300 nm
and high transmission (>95%) for the idler over 5900– temporal walk-off through the 0.5-mm-thick CSP crystal
6700 nm. In the four-mirror OPO cavity (Fig. 1), the are
10 and −70 fs, respectively, much shorter than
focusing mirrors M1 and M2 (radius of curvature of the pump pulse duration of 130 fs, implying excellent
100 mm) and plane mirror M3 were coated on CaF2 sub- temporal overlap among the three interacting waves.
strates for high transmission at the pump (T > 95% at The absolute group-delay dispersions at the pump, signal,
1020–1070 nm) and high reflectivity at the signal wave- and idler wavelengths are 743 fs2 , 532 fs2 , and −250 fs2
length (R > 99.8% at 1.16–1.6 μm). The mirror coating respectively, imposing only a relatively small shaping
was made of an oxide material, which presented a signifi- effect on these pulses.
cant absorption at the idler wavelengths (estimated to be The band edge of CSP is close to 500 nm, implying that
>40% at 5900–6700 nm). The pump beam was tightly fo- pumping near 1000 nm, with broadband high-intensity
cused by a convex lens L1 with a focal length of 50 mm, pulses, may cause TPA. Measuring the transmission of
and had a Gaussian diameter of 60 μm in the position of the e-polarized pump beam through the CSP crystal, we
the CSP crystal. The OPO was singly resonant for the sig- observed that the transmission dropped significantly
nal, which was extracted via a 2% output coupler (OC). with increasing pump intensity, verifying the presence
Since both surfaces of the CSP crystal had a (measured) of TPA. The supporting data, reproduced in Fig. 3,
signal reflection loss of 0.6%, the power extracted from implied a TPA coefficient of 8.3 cm GW−1 for the pump
the OC, with a transmission of 2%, accounted for only pulses, which had durations of 130 fs and a central wave-
45% of the generated signal. The cavity length was ad- length of 1053 nm. In comparison, a TPA coefficient of
justed for synchronism with the 100 MHz repetition rate 2.4 cm GW−1 was reported for pump pulses at a similar
of the pump laser. The idler and residual pump passed central wavelength but with durations of 8.6 ps [13]. This
through M2 and were collimated by an uncoated CaF2 TPA behavior limited the ability to scale the output of
lens L2, followed by an AR-coated Ge window used to the CSP OPO by increasing the pump power; however,
block all the residual pump prior to the idler diagnostics. it did not destabilize the OPO operation, due to the
The high nonlinear coefficient of the CSP crystal and good thermal conductivity of the crystal. In a separate
the extremely high pump intensity enabled by using
femtosecond pump pulses and tight focusing ensure that
an OPO with a thin nonlinear crystal can oscillate at a
moderate average pump power. One benefit of using a
thin nonlinear crystal is the broad phase-matching band-
width. For a CSP crystal with a thickness of 0.5 mm and
at a pump wavelength of 1055 nm, the −3 dB phase-
matching bandwidths for the signal and idler are 28
and 663 nm, respectively. Figure 2 shows phase-matching
efficiency plots for pump wavelengths from 1040 to
1070 nm, which allow signal (idler) tuning from 1285
to 1295 nm (6150–6400 nm).
The other benefit of using such a thin nonlinear crystal
is that the temporal walk-off between the interacting
pulses and their intrapulse group-delay dispersion are
reduced, ensuring good temporal pulse overlap and
limited pulse broadening. Based on the Sellmeier equa- Fig. 3. Transmission through the 0.5-mm-thick CSP crystal as
tions reported in [9], the pump–signal and pump–idler a function of intensity for the e-polarized 130 fs pump pulses.
5112 OPTICS LETTERS / Vol. 38, No. 23 / December 1, 2013

durations of approximately 170 fs. We believe the signal

pulses were slightly chirped, since no dispersion com-
pensation optics were employed, and the round-trip
dispersion of the OPO cavity is estimated to be approx-
imately
930 fs2 , contributed by the CSP crystal and the
slight negative dispersion from the high-reflection mir-
rors. This broad signal bandwidth is due to the broad
pump bandwidth [Fig. 5(b)] and the large phase-matching
bandwidth of the CSP crystal. The incident pump
(dashed line, measured in front of lens L1) and residual
pump (solid line, measured after lens L2) spectra at full
pump power are shown in Fig. 5(b) for comparison. It is
clear that nonlinear frequency conversion occurs over
the full pump spectrum range, confirming the large
phase-matching bandwidth of the thin CSP crystal.
Fig. 4. (a) Measured signal output power from the OC,
Applying the Manley–Rowe relations (assuming signal
residual pump power when the OPO was oscillating, and
residual pump power when the OPO was not oscillating and idler wavelengths of 1275 and 6200 nm, respectively),
versus incident pump power. (b) Measured signal output power the generated idler power is expected to be ∼24 mW.
from the OC versus the absorbed pump power due to OPO However, the idler power after the Ge window was too
oscillation. low to be measured by a thermal power meter with a sen-
sitivity of 0.01 mW. For this reason we believe that nearly
all the generated idler was absorbed by the multilayer
measurement, we confirmed that there was no TPA for oxide coating of the CaF2 mirror. A mirror coated with
similar intensities at the signal wavelength of 1.275 μm. a material (e.g., ZnSe) that is transparent to long-wave
With the 2% OC, the threshold pump power was mid-IR is required to extract most of the generated idler
600 mW. Figure 4(a) shows the signal output power power. Despite this, the 6.2 μm idler after the Ge window
measured after the OC, and the residual pump powers could be detected by a mercury cadmium telluride (MCT)
measured after lens L2 when the OPO was oscillating/ photovoltaic detector operating within the 2–11 μm
blocked. At the maximum pump power of 1.6 W, 0.55 W range. We measured the idler spectrum at full pump
(∼34%) was absorbed due to TPA and residual linear loss power by use of a Fourier-transform infrared (FTIR)
in the CSP crystal, 0.75 W (47%) was transmitted, and spectrometer based on the MCT detector. A He–Ne laser
only 0.30 W (19%) was converted in the nonlinear para- with a central wavelength at 632.8 nm was coupled to the
metric interaction. Figure 4(b) shows the output-coupled interferometer for absolute frequency calibration. As
signal power as a function of the pump power converted shown by the solid line of Fig. 6, the idler spectrum is
by parametric oscillation, indicating an extraction effi- rather broad, with a spectral coverage over 5.8–6.6 μm
ciency of ∼20%. A maximum output-coupled signal (6.2 THz), supporting transform-limited pulses with dura-
power of 53 mW was measured; however, crystal reflec- tions of approximately 160 fs. It is well known that there
tion losses contribute a further 2.4% loss, and therefore is strong absorption by atmospheric water vapor in this
we estimate that the total generated signal power was
118 mW.
The output signal spectrum from the OPO, pumped
at full power, is shown in Fig. 5(a). Its central wavelength
was 1275 nm, with a −10 dB bandwidth of 33 nm
(6.1 THz), supporting transform-limited pulses with

Fig. 6. Solid line: idler spectrum measured by an FTIR spec-

trometer. Dashed line: simulated transmission spectrum
through water vapor, based on the HITRAN database, with a
Fig. 5. (a) Signal spectrum at full pump power. (b) Spectrum water concentration of 1% at one atmospheric pressure, a path
of the incident pump (dashed line) and the residual pump length of 1.4 m, and a resolution (matching experiment) of
(solid line). 2.5 cm−1 (∼10 nm).
 December 1, 2013 / Vol. 38, No. 23 / OPTICS LETTERS 5113

spectral region. The generated idler traveled a path 2. F. Adler, K. C. Cossel, M. J. Thorpe, I. Hartl, M. E. Fermann,
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