Nonlinear response theory with relaxation: The first-order hyperpolarizability
- 11 November 2005
- journal article
- research article
- Published by AIP Publishing in The Journal of Chemical Physics
- Vol. 123 (19), 194103
- https://doi.org/10.1063/1.2107627
Abstract
Based on the Ehrenfest theorem, an equation of motion that takes relaxation into account has been presented in wave-function theory, and the resulting response functions are nondivergent in the off-resonant as well as the resonant regions of optical frequencies. The derivation includes single- and multideterminant reference states. When applied to electric dipole properties, the response functions correspond to the phenomenological sum-over-states expressions of Orr and Ward [Mol. Phys.20, 513 (1971)] for polarizabilities and hyperpolarizabilities of an isolated system. A universal dispersion formula is derived for the complex second-order response function. Response theory calculations are performed on lithium hydride and para-nitroaniline for off-resonant and resonant frequencies in the electro-optical Kerr effect and second-harmonic generation.This publication has 27 references indexed in Scilit:
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