Numerical MCSCF study of the total (electronic and nuclear) parallel polarizability and hyperpolarizability for the H2, HD and D2molecules

Abstract

We present numerical MCSCF calculations of the electronic and nuclear components of the parallel molecular polarizabilities (α zz ) and the second hyperpolarizabilities (γ zzzz ) of H2, HD and D2. Contrary to the H+ 2 case, where the vibrational contribution to γ is fifty times larger than the pure electronic γ, the vibrational γ and the electronic γ for H2 have the same magnitude. The electronic correlation has a stronger effect on α and γ for vibrationally-excited states than for the ground state.