Nonlinear optical properties of organic solids: ab initio polarizability and hyperpolarizabilities of nitroaniline derivatives

The static dipole polarizability, first and second hyperpolarizability tensors of molecules with nonlinear optical characteristics are calculated via ab initio coupled-perturbed Hartree-Fock theory. A study of the effect of basis set augmentation on the calculated properties for the nitrobenzene molecule emphasizes the importance of diffuse functions. The method is then applied to a series of methyl substituted nitroanilines, and comparison with existing experimental data and other computational data is presented. The results indicate that the present approach works well to reproduce experimentally observed trends.