Prediction of Nonlinear Optical Responses of Organic Compounds

The nonlinear optical quantities, second and third harmonics (β and γ), 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 β and γ responses, prior to further investigations of potentially interesting molecules for use in optical materials.