Determination of hyperpolarizability tensor components by depolarized hyper Rayleigh scattering

Depolarized hyper Rayleigh scattering of para-nitroaniline (${\mathit{C}}_{2\mathit{v}}$ symmetry) and nitrocalix[4]arene (${\mathit{C}}_{4\mathit{v}}$ symmetry) in solution has been measured. Using linearly and circularly polarized fundamental radiation information about the ratios between the several hyperpolarizability tensor components, including their sign, was obtained. Results are consistent with the theory developed for both symmetry groups. Comparison between experimental depolarization ratios and ratios obtained from ab initio calculated hyperpolarizability tensor components shows good agreement.