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.