Intra-pulse difference frequency generation in ZnGeP2 for high-frequency terahertz radiation generation.

The highly-nonlinear chalcopyrite crystal family has experienced remarkable success as source crystals in the mid-infrared spectral range, such that these crystals are primary candidates for producing high terahertz frequency (i.e., [Formula: see text] 10 THz) electric fields. A phase-resolved terahertz electric field pulse is produced via intra-pulse difference frequency generation in a chalcopyrite (110) ZnGeP2 crystal, with phase-matching being satisfied by the excitation electric field pulse having polarizations along both the ordinary and extraordinary crystal axes. While maximum spectral power is observed at the frequency of 24.5 THz (in agreement with intra-pulse phase-matching calculations), generation nonetheless occurs across the wide spectral range of 23-30 THz. To our knowledge, this is the first time a chalcopyrite ZnGeP2 crystal has been used for the generation of phase-resolved high-frequency terahertz electric fields.

Generation of 17-32 THz radiation from a CdSiP2 crystal.

A phase-resolved electric field pulse is produced through the second-order nonlinear process of intra-pulse difference frequency generation (DFG) in a (110) CdSiP2 chalcopyrite crystal. The generated electric field pulse exhibits a duration of several picoseconds and contains frequency components within the high-frequency terahertz regime of ∼17-32 THz. The intra-pulse DFG signal is shown to be influenced by single-phonon and two-phonon absorption, the nonlinear phase-matching criterion, and temporal spreading of the excitation electric field pulse. To date, this is the first investigation in which a CdSiP2 chalcopyrite crystal is used to produce radiation within the aforementioned spectral range.

Mid-infrared frequency combs and staggered spectral patterns in χ(2) microresonators.

The potential of frequency comb spectroscopy has aroused great interest in generating mid-infrared frequency combs in the integrated photonic setting. However, despite remarkable progress in microresonators and quantum cascade lasers, the availability of suitable mid-IR comb sources remains scarce. Here, we generate mid-IR microcombs relying on cascaded three-wave-mixing for the first time. By pumping a CdSiP2 microresonator at 1.55 µm wavelength with a low power continuous wave laser, we generate χ(2) frequency combs at 3.1 µm wavelength, with a span of about 30 nm. We observe ordinary combs states with a line spacing of the free spectral range of the resonator, and combs where the sideband numbers around the pump and half-harmonic alternate, forming staggered patterns of spectral lines. Our scheme for mid-IR microcomb generation is compatible with integrated telecom lasers. Therefore, it has the potential to be used as a simple and fully integrated mid-IR comb source, relying on only one single material.

Pump tuning of a mid-infrared whispering gallery optical parametric oscillator.

Optical parametric oscillators (OPOs) constitute an important coherent, narrow-linewidth and widely tunable light source with applications in spectroscopy and many other fields. Their realizations based on whispering gallery resonators (WGRs) provide a small footprint and ultra-low thresholds, with demonstrations of tunability typically done via temperature variation. In this work, we show the pump tuning capabilities of a mm-sized WGR mid-infrared OPO made of CdSiP2. By tuning a telecom wavelength diode laser by 16 nm, we generate tunable light from 2708 to 3575 nm. Furthermore, we show controlled tuning in steps of 1 free spectral range (FSR) and the possibility of 12 GHz of continuous tuning. All these features are in good agreement with the theoretical predictions. We conclude that tuning from 2.4 to 4.9 µm is even possible, while still using commercially available near-infrared diode lasers. This work highlights the advantages of pump tuning of WGR OPOs and provides valuable insights for their precise control.

Seeded optical parametric generation in CdSiP2 pumped by a Raman fiber amplifier at 1.24 µm.

We report a seeded optical parametric generator (OPG) producing tunable radiation from 4.2-4.6 µm. The seeded OPG employs a 13 mm long CdSiP2 (CSP) crystal cut for non-critical phase-matching, pumped by a nanosecond-pulsed, MHz repetition rate Raman fiber amplifier system at 1.24 µm. A filtered, continuous-wave fiber supercontinuum source at 1.72 µm is used as the seed. The source generates up to 0.25 W of mid-infrared (MIR) idler power with a total pump conversion of 42% (combined signal and idler).

Generation of narrowband terahertz radiation via phonon mode enhanced nonlinearities in a BaGa4Se7 crystal.

We report on narrowband terahertz (THz) radiation generation via optical rectification from a BaGa4Se7 crystal. The dense phonon mode distribution of the BaGa4Se7 crystal causes narrow transmission bands in the THz frequency range with enhanced nonlinear susceptibility magnitudes, thus permitting strong narrowband THz radiation generation at the frequencies of 1.97 and 2.34 THz. In comparison to THz radiation generated from a ZnTe crystal, the narrowband THz radiation produced by the BaGa4Se7 crystal is 4.5 times higher at 1.97 THz and 63% higher at 2.34 THz, thus making BaGa4Se7 a viable crystal for use in such areas as security and medicine.

Dependence on excitation polarization and crystal orientation for terahertz radiation generation in a BaGa4Se7 crystal.

Optical rectification is experimentally investigated in a biaxial BaGa4Se7 crystal by considering various combinations of near-infrared excitation polarizations and crystal orientations. The highest terahertz radiation is produced along the Z crystallo-physical direction of the BaGa4Se7 crystal. Despite the optical complexity of the BaGa4Se7 crystal in the terahertz spectral regime, this systematic experimental investigation determines the optimal excitation polarization and crystal orientation for the optical rectification process.

Critically phase-matched Ti:sapphire-laser-pumped deep-infrared femtosecond optical parametric oscillator based on CdSiP2.

We report a high-repetition-rate femtosecond optical parametric oscillator (OPO) for the deep-infrared (deep-IR) based on type-I critical phase-matching in CdSiP2 (CSP), pumped directly by a Ti:sapphire laser. Using angle-tuning in the CSP crystal, the OPO can be continuously tuned across 7306-8329 nm (1201-1369 cm-1) in the deep-IR. It delivers up to 18 mW of idler average power at 7306 nm and >7 mW beyond 8000 nm at 80.5 MHz repetition rate, with the spectra exhibiting bandwidths of >150 nm across the tuning range. Moreover, the signal is tunable across 1128-1150 nm in the near-infrared, providing up to 35 mW of average power in ∼266 fs pulses at 1150 nm. Both beams exhibit single-peak Gaussian distribution in TEM00 spatial profile. With an equivalent spectral brightness of ∼5.6×1020photons s-1 mm-2 sr-10.1% BW-1, this OPO represents a viable alternative to synchrotron and supercontinuum sources for deep-IR applications in spectroscopy, metrology, and medical diagnostics.

High-repetition-rate, deep-infrared, picosecond optical parametric oscillator based on CdSiP2.

We report a high-repetition-rate picosecond optical parametric oscillator (OPO) based on CdSiP2 (CSP) that is synchronously pumped by an Yb-fiber laser at 1064 nm and provides high average power in the deep-infrared (deep-IR) at 79.5 MHz. The OPO is tunable across 6205-6710 nm in the idler, providing as much as 105 mW of average power at 6205 nm and >55 mW over nearly the entire tuning range. The deep-IR idler output exhibits passive power stability better than 2.3% rms over 12 h in good beam quality. The near-IR signal pulses from the OPO have a Gaussian pulse duration of ∼19 ps, measured at 1284 nm. We have investigated the temperature tuning characteristics of the OPO and compared the data with the theoretical calculations using the most recent Sellmeier equations and thermo-optic coefficients for the crystal. To the best of our knowledge, this is the first picosecond OPO based on CSP operating at MHz repetition rates.

Generation of broadband terahertz pulses via optical rectification in a chalcopyrite CdSiP2 crystal.

We report on the generation of broadband (0.07-6 THz) terahertz (THz) radiation via optical rectification in a ⟨110⟩ CdSiP2 (CSP) crystal pumped by a 50 fs, 780 nm central wavelength optical pulse. By measuring the THz phase refractive index and the optical pump group refractive index, good phase matching can be achieved for a crystal thickness ≲200 µm. Due to this crystal's high second order nonlinearity and low absorption losses, it is envisioned that THz generation from CSP could be further enhanced by confining the optical pump pulse to sub-wavelength waveguides.

Pump-tuned deep-infrared femtosecond optical parametric oscillator across 6-7 µm based on CdSiP2.

We report on a high-power femtosecond optical parametric oscillator (OPO) at 80 MHz repetition rate, tunable across 6318-7061 nm in the deep-infrared (deep-IR) using pump wavelength tuning. The OPO, based on CdSiP2 (CSP), is synchronously pumped by a commercial Ti:sapphire-pumped femtosecond OPO in the near-IR, enabling rapid static tuning of the CSP OPO with minimal adjustments to its cavity length. The deep-IR CSP OPO provides as much as 32 mW of average idler power at 6808 nm with spectral bandwidth >1000 nm (at -10 dB level) across the tuning range. By implementing intracavity dispersion control, near-transform-limited signal pulses of ∼100 fs duration with smooth single-peak spectrum are achieved at 1264 nm, corresponding to an idler wavelength at 6440 nm. To the best of our knowledge, this is the first time such practical idler powers in the deep-IR have been generated from a dispersion-compensated CSP femtosecond OPO at sub-100 MHz repetition rate.

Ti:sapphire-pumped deep-infrared femtosecond optical parametric oscillator based on CdSiP2.

We report on a femtosecond optical parametric oscillator (OPO) for the deep-infrared (deep-IR) based on the Kerr-lens-mode-locked Ti:sapphire laser as the pump source. By deploying a novel cascaded intracavity arrangement, comprising a femtosecond OPO based on the nonlinear crystal, CdSiP2, synchronously pumped internal to a MgO:PPLN femtosecond OPO, we have generated broadly tunable radiation across 5958-8117 nm using rapid static cavity delay tuning, with a maximum power of 64 µW at 6791 nm, limited by the absorption in mirror substrates as well as polarization-dependent intracavity losses. The deep-IR idler power exhibits excellent passive stability of better than 1.1% rms over 2 h, with a spectral bandwidth as large as ∼650 nm at ∼6800 nm. The demonstrated concept is generic and can be similarly deployed in other operating time scales and wavelength regions, also using different laser pump sources and nonlinear materials.

High-power femtosecond mid-infrared optical parametric oscillator at 7 µm based on CdSiP(2).

We report a femtosecond optical parametric oscillator (OPO) for the mid-infrared (mid-IR), generating a record average power of 110 mW at 7 µm. The OPO, based on CdSiP(2) (CSP) as the nonlinear crystal, provides idler wavelength tuning across 6540-7186 nm with spectral bandwidths >400 nm at -10 dB level over the entire range, and a maximum bandwidth of 478 nm at 6.9 µm. To the best of our knowledge, this is the highest average power generated from a femtosecond OPO in the deep mid-IR. The OPO also provides near-IR signal wavelengths tunable across 1204-1212 nm with a usable power of 450 mW in 418-fs pulses at 1207 nm. The simultaneously measured signal and idler power exhibit a passive stability better than 1.6% rms and 3% rms, respectively. A mid-IR idler spectral stability with a standard deviation of the frequency fluctuations better than 40 MHz over 15 min, limited by the measurement resolution, is realized. Using the mid-IR idler from the CSP OPO, we perform Fourier-transform spectroscopy to detect liquid phase organic solvent, toluene (C(7)H(8)), in the molecular fingerprint region.

Tunable, high-energy, mid-infrared, picosecond optical parametric generator based on CdSiP2.

We report a tunable, high-energy, single-pass optical parametric generator (OPG) based on the nonlinear material, cadmium silicon phosphide, CdSiP(2). The OPG is pumped by a cavity-dumped, passively mode-locked, diode-pumped Nd:YAG oscillator, providing 25 µJ pulses in 20 ps at 5 Hz. The pump energy is further boosted by a flashlamp-pumped Nd:YAG amplifier to 2.5 mJ. The OPG is temperature tunable over 1263-1286 nm (23 nm) in the signal and 6153-6731 nm (578 nm) in the idler. Using the single-pass OPG configuration, we have generated signal pulse energy as high as 636 µJ at 1283 nm, together with idler pulse energy of 33 µJ at 6234 nm, for 2.1 mJ of input pump pulse energy. The generated signal pulses have durations of 24 ps with a FWHM spectral bandwidth of 10.4 nm at central wavelength of 1276 nm. The corresponding idler spectrum has a FWHM bandwidth of 140 nm centered at 6404 nm.

Compact, 1.5 mJ, 450 MHz, CdSiP2 picosecond optical parametric oscillator near 6.3 µm.

We report a compact, efficient, high-energy, and high-repetition-rate mid-IR picosecond optical parametric oscillator (OPO) based on the new nonlinear material CdSiP(2) (CSP). The OPO is synchronously pumped by a master oscillator power amplifier system at 1064.1 nm, providing 1 µs long macropulses constituting 8.6 ps micropulses at 450 MHz, and it can be tuned over 486 nm across 6091-6577 nm, covering the technologically important wavelength range for surgical applications. Using a compact (∼30 cm) cavity and improved, high-quality nonlinear crystal, idler macropulse energy as high as 1.5 mJ has been obtained at 6275 nm at a photon conversion efficiency of 29.5%, with >1.2 mJ over more than 68% of the tuning range, for an input macropulse energy of 30 mJ. Both the signal and idler beams are recorded to have good beam quality with a Gaussian spatial profile, and the extracted signal pulses are measured to have durations of 10.6 ps. Further, from the experimentally measured transmission data at 1064 nm, we have estimated the two-photon absorption coefficient of CSP to be ß=2.4 cm/GW, with a corresponding energy bandgap, E(g)=2.08 eV.

Optical parametric generation in CdSiP2.

We report efficient generation of picosecond pulses in the near- and mid-IR in the new nonlinear material CdSiP(2) pumped at 1.064 µm by an amplified mode-locked Nd:YVO(4) laser at a 100 kHz repetition rate. By using single-pass optical parametric generation in 8-mm-long crystal cut for type I(e→oo) noncritical phase matching, an average idler power of 154 mW at 6.204 µm together with 1.16 W of signal at 1.282 µm has been obtained for 6.1 W of pump at photon conversion efficiencies of 15% and 23%, respectively. Signal pulse durations of 6.36 ps are measured for 9 ps pump pulses.