Laser induced damage threshold of GaSe with antireflection microstructures at a wavelength of 5 µm.

Large GaSe crystals were grown and various antireflection microstructures (ARMs) were fabricated on their cleaved surfaces using optimized femtosecond laser ablation, which provided the antireflection effect in a wide wavelength range of 4-16 µm. The influence of ARMs created on the GaSe surface on the change of the laser-induced damage threshold (LIDT) of the crystal at a wavelength of 5 µm was evaluated. The 5-µm Fe:ZnMgSe laser with the pulse duration of 135 ns was used for the LIDT test in conditions close to single pulse exposure. The measured values of LIDT of 56 ± 6 MW/cm2 and 51 ± 9 MW/cm2 for two GaSe substrates, respectively, were comparable with the known data of single pulse LIDT of GaSe. The average LIDT intensities of 54 ± 6 MW/cm2 and 52 ± 7 MW/cm2 for the ARMs at two GaSe plates, respectively, were close to LIDT intensities for the corresponding GaSe substrates. The ARMs with lower structural quality had lower LIDT (50-52 MW/cm2) in comparison with the high-quality ARMs (58-60 MW/cm2). High LIDT for high-quality ARMs can be caused by increased selenium content in the ARMs. In any case, all the tested ARMs on the GaSe plates with different surface quality are workable for development of widely tunable mid-infrared nonlinear optical converters.

Antireflection microstructures fabricated on the surface of a LiGaSe2 nonlinear crystal.

LiGaSe2 is a propitious material for nonlinear parametric conversion in the mid-infrared (mid-IR) range. Its refractive index of n = 2.25 in the 2-12 µm wavelength range results in significant losses due to Fresnel reflection. However, the conventional method of increasing the transmittance with antireflection coatings (ARCs) significantly reduces the damage threshold of the material. Fabrication of the antireflection microstructures (ARMs) is an alternative approach for increasing the surface transmittance. In this work, ARMs were fabricated on the surface of a LiGaSe2 crystal using a single-pulse femtosecond laser ablation method. An average transmittance of 97.2% in the 2-8 µm spectral range and the maximum transmittance of 98.6% at 4.1 µm were achieved.

Anisotropic Thermal Expansion and Electronic Structure of LiInSe2.

Optical quality cm-sized LiInSe2 crystals were grown using the Bridgman-Stockbarger method, starting from pure element reagents, under the conditions of a low temperature gradient of 5-6 degrees/cm and a slight melt overheating. The phase purity of the grown crystal was verified by the powder XRD analysis. The thermophysical characteristics of LiInSe2 were determined by the XRD measurements in the temperature range of 303-703 K and strong anisotropy of the thermal expansion coefficients was established. The following values of thermal expansion coefficients were determined in LiInSe2: αa = 8.1 (1), αb = 16.1 (2) and αc = 5.64 (6) MK-1. The electronic structure of LiInSe2 was measured by X-ray photoelectron spectroscopy. The band structure of LiInSe2 was calculated by ab initio methods.

Fabrication of antireflection microstructures on the surface of GaSe crystal by single-pulse femtosecond laser ablation.

GaSe crystals are promising as nonlinear optical converters in the mid- and far-IR ranges. However, it is challenging to increase the GaSe surface transmittance of 77% with conventional antireflection coatings because of poor surface quality, leading to coating adhesion problems. Antireflection microstructures (ARMs) offer an alternative way of increasing surface transmittance. In this work, ARMs were fabricated on the surface of a GaSe plate by single-pulse femtosecond laser ablation. An average GaSe surface transmittance of 94% in the 7-11 µm range and a maximum transmittance of 97.8% at 8.5 µm were obtained. The proposed method can be used to increase the efficiency of GaSe-based nonlinear converters.

Thermo-optic dispersion formula for LiGaS2.

This paper reports on new experimental results on the temperature-dependent phase-matching properties of LiGaS2 for second-harmonic generation and sum-frequency generation in the 0.820-10.5910 µm spectral range. In addition, we present a thermo-optic dispersion formula that provides a good reproduction of the present experimental results when combined with the Sellmeier equations presented in our previous paper, Kato et al. [Opt. Lett.42, 4363 (2017)OPLEDP0146-959210.1364/OL.42.004363].

Phase-matching properties of LiGaS2 in the 1.025-10.5910 µm spectral range.

This Letter reports on the new experimental results for second-harmonic generation and sum-frequency generation in LiGaS2 in the 1.025-10.5910 µm range, together with the new Sellmeier equations, which provide a good reproduction of the present experimental results, as well as the published data points for a Ti:Al2O3 laser (λ=0.8200 µm)-pumped optical parametric amplifier in the 3.7434-11.0079 µm range and a Nd:YAG laser-pumped optical parametric oscillator at ∼5.457 µm.

Structures and optical properties of two phases of SrMgF4.

SrMgF4 has an extremely large bandgap Eg of 12.50 eV as obtained from reflection dispersion. The symmetry of this crystal is monoclinic P21 at room temperature and transforms to the orthorhombic Cmc21 phase near 478 K as the temperature increases. The acentric character of the low-temperature (LT) phase is confirmed by pyroelectric luminescence at T < 440 K. The fundamental absorption edge of the LT phase is located at 122 nm (10.15 eV). A considerable difference between the absorption edge and bandgap Eg is due to the strong exciton absorption. The first-principles electronic structure, refractive indices, nonlinear susceptibility and polarizability were calculated for both LT and high-temperature (HT) phases. Band-to-band transitions are direct for the LT phase but indirect for HT. In spite of relatively low birefringence (∼0.017) and nonlinear susceptibility (∼0.044 pm V(-1), an order lower than that in KDP), SrMgF4 crystals are considered promising for nonlinear optics thanks to their transparency far in the vacuum ultraviolet spectral region.

Thermophysical properties of lithium thiogallate that are important for optical applications.

Lithium thiogallate LiGaS2 is one of the most common nonlinear crystals for mid-IR due to its extreme beam strength and wide transparency range; however, its thermophysical properties have not yet been practically studied. Large crystals of high optical quality are grown. DTA revealed features at 1224 K below melting point (1304 K) that are associated with the oxygen containing compounds of the LiGaO2-x S x type. The thermal conductivity of LiGaS2 (about 10.05 W (m-1 K-1)) and band gap value (3.93 eV at 300 K) are found to be the highest in the LiBC2 family. Isotropic points in the dispersion characteristics for the refractive index are found and LiGaS2-based narrow-band optical filters, smoothly tunable with temperature changes, are demonstrated. Intense blue photoluminescence of anionic vacancies V S is observed at room temperature after annealing LiGaS2 in vacuum, whereas orange low-temperature emission is related to self-trapped excitons. When LiGaS2 crystals are heated, spontaneous luminescence (pyroluminescence) takes place, or thermoluminescence after preliminary UV excitation; the parameters of traps of charge carriers are estimated. The obtained data confirm the high optical stability of this material and open up prospects for the creation of new optical devices based on LiGaS2.

Nd:YAG pumped nanosecond optical parametric oscillator based on LiInSe2 with tunability extending from 4.7 to 8.7 microm.

LiInSe(2) is one of the few (only 5) non-oxide nonlinear optical crystals whose band-gap (2.86 eV) and transparency allowed in the past nanosecond optical parametric oscillation in the mid-IR without two-photon absorption for a pump wavelength of 1064 nm. However, the first such demonstration was limited to the 3.3-3.78 microm range for the idler and the average idler power did not exceed 2.5 mW. Here we report broadly tunable operation, from 4.7 to 8.7 microm, of an OPO based on LiInSe(2), achieving maximum idler pulse energy of 282 microJ at approximately 6.5 microm, at a repetition rate of 100 Hz (approximately 28 mW of average power).

LiInSe2 nanosecond optical parametric oscillator.

Optical parametric oscillation using the new lithium selenoindate nonlinear crystal is reported for what is to our knowledge the first time. A 17 mm long, type II phase-matched sample is pumped by a 10 ns Nd:YAG laser. The minimum pump energy threshold is 3 mJ for a signal-resonant configuration. The signal and idler waves are tunable between 1.47 and 1.57 microm, and 3.3 and 3.78 microm, with a total output energy of 170 microJ corresponding to a 2.4% energy conversion at 8 mJ pump, only limited by the AR coatings damage. With optimized crystal quality and coatings, lithium selenoindate should show superior performance as compared with AgGaS(e)2 crystals, owing to its 4x larger thermal conductivity.

Widely tunable continuous-wave mid-infrared radiation (5.5-11 microm) by difference-frequency generation in LiInS2 crystal.

The first demonstration, to the best of our knowledge, of continuous-wave (cw) difference-frequency generation (DFG) in LiInS2 crystal is reported. Wide spectral coverage (5.5-11.3 microm) has been obtained with angle and wavelength tuning for type II (eoe) critically phase-matched parametric interaction. The phase-matching conditions in cw DFG have been investigated, which allowed us to improve the Sellmeier parameters by use of a two-pole dispersion equation. An effective nonlinear coefficient deff = 6.9 +/- 0.8 pm/V has been determined at approximately 7 microm relative to the well-known nonlinear coefficient d36 of AgGaS2, which yields a power-conversion efficiency of approximately 12.4 microW/(W2 cm). We evaluated the high-resolution spectral characteristics of the DFG source by recording C2H2 and SO2 spectra.