Polarizabilities and Hyperpolarizabilities of Small Polyatomic Molecules in the Uncoupled Hartree–Fock Approximation

Near Hartree–Fock LCAO–MO–SCF contracted Gaussian wavefunctions are used to calculate the polarizabilities and hyperpolarizabilities of water, methane, carbon monoxide, and formaldehyde. The polarizabilities are shown to be in good agreement with the experimental data. In the case of water, an attempt was made to use the calculated hyperpolarizabilities to predict the line intensities and the depolarization ratio of a double quantum scattering experiment. Unfortunately, direct comparison with the actual experiment is premature at this time due to ambiguities in the interpretation of the experimental results.