On the Contribution of Mixed Terms in Response Function Treatment of Vibrational Nonlinear Optical Properties

Abstract

A new response theory formulation for calculating second-order vibrational nonlinear optical properties has recently been 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