Abstract

The dispersion of the first molecular hyperpolarizability β of strongly charge-transfer chromophores is investigated. In the two-photon resonance regime, both dephasing and vibronic structure plays an important role in affecting the molecular hyperpolarizability An equation for β that includes the effect of dephasing and vibrational structure of electronic states is derived. It is shown that, if only the dephasing mechanism is included in the two level model, the intrinsic hyperpolarizability β 0 calculated from the hyper-Rayleigh scattering (HRS) experimental data using the Oudar-Chemla equation, will decrease with decreasing the excitation wavelength. The trend is reversed when the vibrational structure is also incorporated.

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