Prediction of nonlinear optical responses of organic compounds.

The nonlinear optical quantities, second and third harmonics (beta and gamma), were predicted using a quantitative structure-property relationship (QSPR) approach. Molecular orbital ab initio calculations were applied to generate easily accessible variables to be used in the partial least-squares analysis. Simplified equations are presented that could be used to predict the experimental beta and gamma responses, prior to further investigations of potentially interesting molecules for use in optical materials.