title: Nonlinear response theory with relaxation: the first-order hyperpolarizability.
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.
authors.affiliation: Department of Physics, Chemistry and Biology, Linköping University, SE-581 83 Linköping, Sweden. panor@ifm.liu.se
authors.forename: Patrick
authors.initials: P
authors.lastname: Norman
authors.forename: David M
authors.initials: DM
authors.lastname: Bishop
authors.forename: Hans Jørgen Aa
authors.initials: HJ
authors.lastname: Jensen
authors.forename: Jens
authors.initials: J
authors.lastname: Oddershede