Dispersion of the hyperpolarizability of the carbon tetrachloride molecule

The second hyperpolarizability of a molecule is the microscopic version of the third order susceptibility. Direct measurements of the ratio of the second hyperpolarizability of carbon tetrachloride to diatomic nitrogen are made possible through electric field induced second harmonic generation. Whenever the dispersion of the second hyperpolarizability is not negligible, there should be deviations from Kleinman symmetry. Previous experimental data for second hyperpolarizability of this molecule have only been at two frequencies and theory predicts the zero frequency value. In order to provide for a better extrapolation to zero frequency, additional gas phase measurements of this ratio at optical frequencies are presented and discussed