Effect of vibration on the linear and nonlinear optical properties of HF and (HF)2

Abstract

Electronic and vibrational contributions to the linear and nonlinear optical properties of the HF dimer have been calculated for the first time. The vibrational components are very significant with mechanical anharmonicity effects, as determined by perturbation-theoretic formulas, playing a major role. We identify the important anharmonic potential constants and analyze the validity, as well as the possible extension, of our theoretical treatment. Parallel computations, for purposes of comparison, have also been performed for the monomer.