Direct-Resolvent-Operator Computations on the Hydrogen-Molecule Dynamic Polarizability, Rayleigh, and Raman Scattering

Abstract

Direct sum-over-states methods are used to evaluate the frequency-dependent polarizability and anisotropy for ground-state ${\mathrm{H}}_2$. Rayleigh and rotational and vibrational Raman cross sections for photon scattering and depolarization ratios are given for Lyman-$\alpha$ radiation. An assessment of the accuracy obtainable by the direct use of sum-over-states methods indicates its high promise as a technique for accurate computation of molecular properties. The Dalgarno—Epstein [J. Chem. Phys. 50, 2837 (1969)] technique for obtaining a finite-set representation of components of the resolvent operator is shown to be effective for molecules.