Gas phase hyper-Rayleigh scattering measurements

摘要

Measurements of hyper-Rayleigh scattering intensities and polarization ratios are presented for nine small molecules in the gas phase [CH_4, CF_4, CCl_4, N_2O, NH_3, D_2O, SO_2, CF_2Cl_2, and (CH_3)_2CO]. In four cases [CH_4, CF_4, CCl_4, and N_2O] all molecular hyperpolarizability tensor components can be determined from the measurements. The results of this experiment are compared with the results of previous ab initio calculations, finding discrepancies up to 60%. Including vibrational contributions decreases the discrepancies for CH_4 and CF_4 and increases them for CCl_4, D_2O, and NH_3.