Dispersion formulas for the second hyperpolarizability components

Christof Hättig
Department of Chemistry, Århus University, DK-8000 Århus C, Denmark

Chem. Phys. Lett, 296 (1998) 245-252
(Received 22 June 1998; in final form 17 August 1998)

The frequency-dependence of the isotropic parallel avarage of the second hyperpolarizability can be expanded in a compact way using dispersion coefficients, which are independent of the optical process, if three effective frequencies are introduced. We propose similar expansions for the second hyperpolarizability components gamma_orthogonal and gamma_Kerr and give explicit expressions for the hyperpolarizability dispersion coefficients in terms of derivatives of the hyperpolarizabilities with respect to their frequency arguments. The relation of the hyperpolarizability dispersion coefficients and the Cauchy moments of linear response theory is discussed and comparison is made with previously proposed dispersion formulas.


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