CdSiP2 crystals with sizes and optical quality suitable for use as nonlinear optical devices are disclosed, as well as NLO devices based thereupon. A method of growing the crystals by directional solidification from a stoichiometric melt is also disclosed. The disclosed NLO crystals have a higher nonlinear coefficient than prior art crystals that can be pumped by solid state lasers, and are particularly useful for frequency shifting 1.06 μm, 1.55 μm, and 2 μm lasers to wavelengths between 2 μm and 10 μm. Due to the high thermal conductivity and low losses of the claimed CdSiP2 crystals, average output power can exceed 10 W without severe thermal lensing. A 6.45 μm laser source for use as a medical laser scalpel is also disclosed, in which a CdSiP2 crystal is configured for non-critical phase matching, pumped by a 1064 nm Nd:YAG laser, and temperature-tuned to produce output at 6.45 μm.