FREQUENCY-DEPENDENT HYPERPOLARIZABILITIES OF HALOFORMS FROM ABINITIO SCF CALCULATIONS

Ab initio calculations of the frequency-dependent polarizabilities and first and second hyperpolarizabilities of the haloform series have been performed within the framework of the time-dependent coupled perturbed Hartree-Fock method. Dynamic polarizabilities show reasonably good agreement with available experimental data. The theoretical value of β(SHG) for CHF3 is in excellent agreement with the experiment gas phase data. A large discrepancy is noted between theory and experiment for the other molecules both for β and γ. For CHI3, the magnitude of γ and its dispersion are large, in accord with experiment. © 1990.