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We report some recent results on thick heteroepitaxial growth of GaP on GaAs substrates and on orientation-patterned (OP) GaAs templates conducted in a hot-wall horizontal quartz reactor for Hydride Vapor Phase Epitaxy. The growths on the plain substrates resulted in up to 500 µm thick GaP with smooth surface morphology (RMS

Quasi-phase-matched (QPM) GaP layers up to 300 μm thick have been produced by low-pressure hydride vapor phase epitaxy (LP-HVPE) overgrowth on orientation-patterned GaAs (OPGaAs) templates fabricated using a wafer-fusion bonding technique. The growth on the OPGaAs templates resulted in up to 200 μm thick vertically propagating domains, with a total GaP thickness of 300 μm. The successful thick growth on OPGaAs templates is the first step towards solving the material problems associated with unreliable material quality of commercially available GaP wafers and making the whole process of designing QPM frequency conversion devices molecular beam epitaxy free and more cost-effective.

Frequency conversion in orientation-patterned (OP) materials is a leading approach for generating mid- and long-wave IR radiation. Although several phase-matching and quasi-phase-matching (QPM) materials have been investigated to date none of these have met all requirements for power, tunability and frequency range of the pursuit applications. We present an original approach that successfully combines in a QPM heterostructure two of the most promising materials, GaP—a material with lower two and three-photon absorption than GaAs, and GaAs—a material with a mature process for fabrication of high quality OP templates. Up to 300 µm thick OPGaP with excellent domain fidelity has been repeatedly grown with 100 µm/h by hydride vapor phase epitaxy on the robust and high quality OPGaAs templates. Some simplifications of both template fabrication and growth process are also reported. The samples, characterized by AFM, SEM, XRD, EDS and TEM, showed smooth surface morphology and high crystalline quality. Special attention was paid to the interface and especially to the mechanism of forming an intermediate ternary transition layer. This led to determining certain criteria that indicate, which other heteroepitaxial cases would be also successful. Thick growths of GaAsP and GaP on other alternative substrate materials by combining a-close-to-equilibrium with a-far-from-equilibrium processes were also performed. Efforts to develop heterostructures in horizontal and vertical direction have been also made. The success with one less favorable (in point of view of lattice mismatch) case, presented here, indicates that we should have even better results in other cases with closer lattice matches.

Thick hydride vapor phase epitaxially grown orientation-patterned gallium phosphide (OPGaP) is a leading material for quasi-phase matching (QPM) frequency conversion in the mid- and longwave infrared (IR). This is due to its negligible two-photon absorption (2PA) in the convenient pumping range 1 – 1.7 μm, compared with the 2PA of some traditional QPM materials, such as GaAs. In this paper, we describe homo- and heteroepitaxial growth techniques aimed to produce hundreds of microns thick OPGaP on: 1) OPGaAs templates fabricated using an improved wafer-fusion process; 2) OPGaAs templates fabricated by using a molecular beam epitaxy (MBE) for sublattice polarity inversion, but one with and one without MBE regrowth after the inversion. Some of the advantages of the heteroepitaxial growth of OPGaP on OPGaAs templates include: 1) achieving good domain fidelity as a result of the significantly higher OPGaAs template quality; 2) eliminating the needs of using the poor quality commercially available GaP in the production of thick OPGaP material, and 3) suppression of the additional absorption band between 2 – 4 μm (which is due to incorporation of n-type impurities) and, in general, improvement of the IR transmittance in the entire IR region. Combining the advantages of the two most promising nonlinear materials, GaAs and GaP, will accelerate the development of high power, broadly tunable laser sources in the IR which, in addition, will be offered with higher device quality and at a reasonably lower unit cost.

Coherent sources that are broadly and continuously tunable in the mid- and longwave infrared are of interest for a variety of scientific, commercial, and military applications. The advantages in an OPO of quasi-phasematched materials like orientation-patterned gallium arsenide (OPGaAs) come at the cost of the angle tuning possible in birefringent nonlinear crystals. Temperature tuning is limited by the material’s dn/dT value, and lacks speed and stability. A better alternative is to tune the OPO by tuning the pump laser. Here we report an OPGaAs OPO pumped by a gain-switched Cr:ZnSe laser which was continuously tuned by an intracavity etalon. The etalon also narrowed the output linewidth to around 4 nm. The Cr:ZnSe laser operated at a repetition rate of 500 Hz with a 45 ns pulsewidth. The pump was focused to a spot size (1/e2) of 100 μm at the center of a simple linear resonator formed by two 5-cm ROC mirrors. The OPGaAs crystal was 14 mm long, with a period of 97 μm, and was mounted with no active cooling. Tuning the pump laser over a range of 90 nm (2385-2475 nm) produced OPO output over a range of almost 4.5 μm (3500-7450 nm). OPO tuning was ultimately limited by coatings on the crystals and the resonator mirrors, as the Cr:ZnSe laser is capable of much broader tuning as a pump source. A maximum slope efficiency of 21% was obtained, with a pulse energy threshold of 84 μJ.

This article presents recent results related to development of thick quasi-phase-matched GaP for incorporation in high power sources radiating in the mid-infrared. The focus was on increasing the growth rate and layer thickness of orientation patterned GaP, while ensuring equal vertical deposition rates and rectangular shape of the domain mesas for both opposite crystallographic lattice orientations. Additionally, we present solutions which confine the presence of uncontrollable hillock growth. The experiments were conducted in a hot-wall horizontal quartz reactor using a standard low-pressure hydride vapor phase epitaxial (HVPE) process. GaP was grown on bare, half-patterned (HP) and orientation-patterned (OP) templates fabricated on (100) GaP and (100) misoriented 4° towards (111)B substrates. The domains were oriented either along the [011] or the [011] direction. We compared a sub-lattice inversion MBE assisted process and a wafer fusion bonding technique to create OP templates. When the growth was performed on bare material, the properly chosen growth conditions resulted in reproducible growth of up to 370 μm thick layers with high optical, surface and structural quality, grown at a growth rate of 100 μm/h in one-hour long experiments and 45 μm/h for 8-h long growths. The presence of a core inside the hillocks growing on the layer surface was eliminated. The hillocks were flattened and widened, which allowed often a single hillock to span several domains with alternating opposite crystallographic orientations, when growth was performed on patterned templates. The HP templates were used to determine the optimal substrate and pattern orientations prior to starting growth experiments on OP-templates. As an additional result they revealed that growth could be hillock-free for certain orientations. Growths on OP templates achieved stable growth rates of 50–70 μm/h with domain walls propagating vertically. The growth followed the periodicity of the initial pattern. The maximal thickness achieved to date on OP GaP is about 350 μm.

Nonlinear optical frequency conversion is an effective technique for generating infrared (IR) and terahertz (THz) wavelengths not readily available from existing laser sources. Birefringent materials such as LiNbO3 are often used to generate wavelengths where gaps exist, but are unsuitable in the mid-IR, far-IR, and THz regions as these materials are often opaque in these regions. As an alternative, GaAs has been employed for frequency conversion in these regions using quasi-phase-matching (QPM) to overcome the material’s lack of birefringence. QPM has been successfully demonstrated in GaAs using fused stacks of thin alternately oriented layers or inverted orientation patterned (OP) grating templates overgrown with thick columnar GaAs layers. Although GaAs has a high nonlinear coefficient d14 = 170 pm/V at 1.064 μm and good thermal conductivity (52 W/m K), it suffers from strong two-photon absorption below 1.7 μm making it inefficient when pumped with a source less than or equal to this wavelength. GaP also has a high nonlinear coefficient d14 = 71 pm/V at 1.064 μm, better thermal conductivity (110 W/m K) and much lower two-photon absorption in the 1 μm region. Therefore, OPGaP is desirable for NLO applications in the mid-IR and THz that use commercially available pump lasers in the 1.06–1.55 μm wavelength range. In this work the fabrication of OPGaP templates suitable for thick columnar hydride vapor phase epitaxial growth of GaP is reported using a commercially viable wafer fusion technique.

We have grown and characterized thick zinc selenide (ZnSe) films up to millimeter thickness on unpatterned gallium arsenide (GaAs) wafers and orientation-patterned substrates by physical vapor transport. The patterns were designed to achieve alternating [0 0 1] and [0 0 1¯] orientations. The quality of the films was evaluated by X-ray diffraction, scanning electron microscopy (SEM), and anisotropic etching to determine the morphology and crystallinity. ZnSe films grew epitaxially on the templates and X-ray rocking curves showed full widths at half maximum (FWHM) less than 0.2°. Orientation-patterning up to hundreds of microns film thickness was verified by SEM and etching profiles.

Optical parametric oscillators (OPOs) producing longwave output from a much shorter pump wavelength suffer from low conversion efficiency into the idler due to the large quantum defect compared with similar devices operating in the 3 – 5 μm regime. One method to increase pump to idler conversion efficiency is to recycle the undesired and higher energy signal photons into additional idler photons in a second nonlinear stage. We present numerical simulation results showing the improvement in efficiency that can be obtained in a linear, two stage, cascaded orientation patterned gallium arsenide (OPGaAs) nanosecond OPO. It includes diffraction, crystal loss, phase mismatch, pump depletion, and back conversion; and it assumes monochromatic waves but it neglects group velocity dispersion. For a singly resonant oscillator (SRO) pumped by a 2.054 μm Tm:Ho,YLF laser with 45 ns pulse widths, the addition of the second crystal in the cavity increases idler generation by overall factor of two and exceeds the quantum defect limit. The model has been validated by comparison with SNLO for the case of a single-stage OPO, and suggests crystal and resonator parameters that will lead to an optimized cascaded OPO.

A series of nonlinear materials including GaAs, GaP, and ZnSe have been examined to determine their suitability for non-linear frequency conversion devices (FCD) and more specifically their use as high power, compact and broadly tunable IR and THz sources for defense and security applications. The more mature GaAs was investigated to reveal the causes for the optical losses that restrict achievement of higher conversion efficiency in quasi-phasematched FCD, while the efforts with GaP were oriented in developing simple, cost effective techniques for fabrication of orientation patterned (OP) templates and optimizing the subsequent thick HVPE growth on these templates. Thus, average growth rates of 50- 70 μm/h were achieved in up to 8-hour long experiments. High optical layer quality was achieved by suitable control of the process parameters. The optimal orientation of the pattern was determined and used as essential feedback aiming to improve the template preparation. This led to the production of the first 300-400 μm thick device quality OPGaP. Efforts to suppress the parasitic nucleation during growths with longer duration or to achieve thicker layers by a 2 step growth process were also made. The main challenge with the newer candidate, OPZnSe, was to establish suitable regimes for hydrothermal growth on plain (001) ZnSe seeds grown by chemical vapor deposition. Two different temperature ranges, 330-350 °C and 290-330 °C, were investigated. The mineralized concentration was also manipulated to accelerate the growth in (111) direction and, thus, to improve the growth in (001) direction. The next material in the line is GaN. The traditional HVPE approach will be combined with a growth at low reactor pressure. Growths will be performed in the next sequence: growth on thin GaN layers grown by MOCVD on sapphire wafers, growth on half-patterned GaN templates with different orientations and, finally, growth on OPGaN templates.

Hydride vapor phase epitaxial growth of thick GaP was performed on plain substrates and on half-patterned templates in order to determine the favorable pattern orientations and the optimal growth conditions for thick device quality orientation patterned GaP. Initial optical characterization and testing of frequency conversion in the grown OPGaP are in progress.

Progress in developing a cost effective technique for fabrication of orientation patterned GaP templates and a reliable technology for thick epitaxial growth on them is described. First 350 μm thick device quality OPGaP is produced.

For the first time thick orientation-patterned GaP (OPGaP) was repeatedly grown heteroepitaxially on OPGaAs templates as a quasi-phase matched medium for frequency conversion in the mid and longwave IR, and THz regions. The OP templates were fabricated by wafer-bonding and in a MBE-assisted polarity inversion process. Standard low-pressure hydride vapor phase epitaxy (LP-HVPE) was used for one-step growth of up to 400 µm thick device quality OPGaP with excellent domain fidelity. The presented results can be viewed as the missing link between a well-developed technique for preparation of OP templates, using one robust nonlinear optical material (GaAs), and the subsequent thick epitaxial growth on them of another material (GaP). The reason for these efforts is that the second material has some indisputable advantages in point of view of thermal and optical properties but the preparation of native templates encounters challenges, which makes it difficult to obtain high quality homoepitaxial growth at an affordable price. Successful heteroepitaxial growth at such a relatively high lattice mismatch (- 3.6%) in a close to equilibrium growth process such as HVPE is noteworthy, especially when previously reported attempts, for example, growth of OPZnSe on OPGaAs templates at about 10 times smaller lattice mismatch ( + 0.3%) have produced only limited results. Combining the advantages of the two most promising nonlinear materials, GaAs and GaP, is a solution that will accelerate the development of high power, tunable laser sources for the IR and THz region, which are in great demand on the market.

Halide vapor phase epitaxial growth of GaP was performed on GaP half- and orientation — patterned templates. This allowed optimization of substrate material, patterning approach and pattern orientation, which resulted in growth of +350 μm thick quasi-phase matched GaP with successful replication of the initial patterns.

Coherent mid-IR sources based on orientation-patterned GaAs (OPGaAs) are of significant interest in diverse scientific, medical, and military applications. The generation of long-wavelength mid-IR beams in OPGaAs using optical parametric oscillation exhibits limitations in the obtainable pulse energy and peak power. The master oscillator power amplifier concept is demonstrated in OPGaAs, by which a mid-IR source based on optical parametric oscillation can be scaled to high energy by amplification of the output of the optical parametric oscillator in an optical parametric amplifier (OPA). A fivefold increase in the pulse energy is obtained using this method by amplifying 3.85μm pulses in an OPGaAs OPA pumped by a Th,Ho:YLF Q-switched laser.

The U.S. Air Force is developing orientation-patterned GaAs (OPGaAs) for nonlinear frequency conversion in the 2-5 μm and 8-12 μm regions. We report recent progress in OPO device performance which reflects continued improvement in material quality. Seven new OPGaAs samples, representing four distinct growth regimes, were evaluated in terms of threshold, slope efficiency, and output spectral content using a Q-switched Tm,Ho:YLF laser operating at 2 μm as the pump source. The samples were identical in base template, grating period, length, and AR coating, permitting direct comparison of results to identify favorable growth conditions. As anticipated, performance varied significantly among the sample set, with slope efficiencies from 12% to 35% and thresholds from 9 μJ to 40 μJ. Less anticipated was the low level of uniformity across each sample and between samples grown in the same growth run. Significant variations in slope efficiency and threshold were not uncommon. Still, most of the samples performed manifestly better than previously grown material, indicating an overall improvement in OPGaAs quality. Research continues on understanding growth processes, optical loss mechanisms, and how these translate into device performance.

Orientation-patterned GaP is a promising nonlinear material for frequency conversion in the mid and longwave IR (2-5 µm and 8-12 µm) by quasi-phase matching. As an alternative to OPGaAs, OPGaP has the advantage of having lower two-photon absorption in the convenient pumping range 1 – 1.7 µm. We report recent results on development of thick QPM GaP for high power tunable laser sources radiating in the mid IR. Two are the major challenges to producing OPGaP: development of simple techniques for preparation of patterned templates and a technology for fast epitaxial growth of thick, high quality GaP on these templates. The focus was to adapt/simplify the wafer fusion process for OPGaP template preparation. Then increase the growth rate and layer thickness of regrown material, while maintaining vertical domain propagation. The growth experiments were conducted in a horizontal quartz reactor, using a standard hydride vapor phase epitaxial process. The growth was performed on: (i) plain (100) GaP; (ii) half-patterned (HP) and (iii) orientation-patterned (OP) templates, fabricated on (100) GaP. Up to 370 µm thick layers with high crystal and optical quality were reproducibly grown on plain material. Growth on HP templates resulted in up to 470 µm thick layers with rectangular mesa‟s shape. These results were used to determine the optimal substrate and pattern orientations. HVPE growth on OP templates achieved stable growth rates of 50-70 µm/h with domain walls propagating vertically, following the periodicity of the initial pattern, and resulted in the first 350 µm thick device quality OPGaP.

Orientation-patterned GaAs (OPGaAs) shows great promise as a nonlinear optical material for frequency conversion in the 2-5 micron and 8-12 micron regions. We report recent progress in each of the three main areas of OPGaAs development: fabrication of patterned templates using a combination of wafer bonding and MBE techniques; thick-layer HVPE growth; and material and OPO device characterization. This work has led to significant improvements in material quality, specifically reduced optical loss, increased sample thickness, improved patterned domain fidelity, and greater material uniformity. Advances in material quality have in turn enabled demonstration of OPO devices operating in the 3-5 micron spectral region. Optical loss and OPO performance measurements on a series of OPGaAs samples are presented, with the goal of understanding how these properties are influenced by growth conditions, and how OPO performance may be improved. Research continues on understanding loss mechanisms, correlating performance with material properties, transitioning the technology into an industrial process, and extending it to additional materials.

OPO performance in 2-micron-pumped OPGaAs samples grown on different templates was found to be comparable, but exhibited significant variation within and between samples. Measured signal and idler wavelength values agreed closely with theory.

We report a Cr2+:ZnSe face-cooled disk laser pumped by a 1.9 μm Tm fiber laser. Direct modulation of the fiber laser permitted operation of the Cr laser at repetition rates from true CW to 1 kHz, with slope efficiencies up to 28% and thresholds as low as 200 mW, performance comparable to the case of Q-switched pumping.

We have demonstrated a target ranging and identification technique based on the timing modulation of a mode-locked laser coupled with fast incoherent detection. The range-to-target and the target-depth information have been determined with a resolution of better than 25 cm at single-pulse signal-to-noise ratios below 0.1. Our modeling results suggest that laser average power requirements remain a challenge, with upwards of 100 W likely needed for extension of this technique to ranges over 10 km, but improvements in overall system throughput would allow realization of its potential.

We have demonstrated a target ranging and identification technique based upon timing-modulation of a mode-locked laser coupled with a fast detector. Range -to-target and target depth information have been determined, with a resolution of better than 25 cm at signal-to-noise ratios below 0.01. Modeling suggests that laser average power requirements remain a challenge, with upward of 100 W likely needed for extension of this technique to ranges over 10 km, but improvements in overall system throughput would allow realization of its potential.

Damage thresholds at 2 μm exceeding 10 J/cm2 were measured in ZnGeP2 witness samples representing a range of growth runs and surface treatments. Samples grown more recently were more robust, but clear correlations between damage properties and surface quality, coating type, or incident polarization were not observed. Variation in damage threshold both within individual samples and between samples was quite large. Comparison with uncoated diffusion-bonded and single-wafer GaAs shows that uncoated ZnGeP2 damages at slightly lower energy density than does GaAs (approximately 4 J/cm2 versus 5.5 J/cm2, respectively).