THEORETICAL INVESTIGATION OF THE NONLINEAR OPTICAL-PROPERTIES OF H-2 AND D2 - EXTENDED BASIS SET

Calculations are reported of the dynamic second hyperpolarizabilities (gamma) of H2 and D2 which are relevant to three different nonlinear optical processes. They have been carried out using an expanded basis set for the DELTA-states that occur in the sum-over-states formula. There is extremely good agreement with recent electric-field-induced second-harmonic-generation experiments; e.g., the experimentally derived static, averaged, gammaBAR parallel-to (electronic) for H2 is 686 +/- 4 e4a0(4)E(h)-3, whereas our value is 683 e4a0(4)E(h)-3. Values of the dynamic B and C polarizabilities are also given.