On the contribution of mixed terms in response function treatment of vibrational nonlinear optical properties

摘要

A new response theory formulation for calculating second-order vibrational nonlinear optical properties has been recently presented by Hansen et al., J Chem Phys, 2009, 131, 154101. For so-called mixed terms, this method contains a correction to account for an approximation made in the classic Bishop and Kirtman, J Chem Phys, 1991, 15, 2646 perturbation treatment. This correction vanishes in the static limit and is here shown to vanish also in the high-frequency limit. The response theory formulation is extended to third-order properties and, in that case, vanishes in both limits as well.