A layered OP material is provided that comprises an OPGaAs template, and a layer of GaP on the OPGaAs template. The OPGaAs template comprises a patterned layer of GaAs having alternating features of inverted crystallographic polarity of GaAs. The patterned layer of GaAs comprises a first feature comprising a first crystallographic polarity form of GaAs having a first dimension, and a second feature comprising a second crystallographic polarity form of GaAs having a second dimension. The layer of GaP on the patterned layer of GaAs comprises alternating regions of inverted crystallographic polarity that generally correspond to their underlying first and second features of the patterned layer of GaAs. Additionally, each of the alternating regions of inverted crystallographic polarity of GaP are present at about 100 micron thickness or more. A method of forming the OPGaP is also provided.