Abstract

The first hyperpolarizabilities (β) of donor–acceptor-substituted push–pull molecules are generally described by a model in which the lowest excited electronic state dominates the optical response. It is shown that within the usual assumptions accompanying this two-state model, β(-2ω; ω, ω) can be expressed in terms of a Kramers–Kronig transform of the linear optical absorption spectrum. The method is applied to p–nitroaniline and several other push–pull chromophores, and results are compared with experimental data where available. Comparison of calculated and measured frequency dispersions is suggested as a purely experimental method, requiring no additional parameters, to test the assumptions of the two-state model.

© 2002 Optical Society of America

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