Abstract
The calculations of the first hyperpolarizability frequency dispersion effect of hemicyanine derivative chromophore have been performed employing time-dependent Hartree-Fock and sum-over-states method respectively. Two-photon resonance enhancement characteristics of second harmonic generation β(-2ω；ω，ω) have also been investigated using the two-level model (TLM), which was originated by Ouder and Chemla. The results indicate that the first excited state dominates the nonlinear optical properties of hemicyanine derivatives. The first hyperpolarizability β(-2ω；ω，ω) increases with the decrease of fundamental wavelength and gives rise to two-photon resonance near the fundamental wavelength of 950 nm, in accordance with the known experimental facts. In addition, the relaxation effect of the excited states should be considered for TLM in the resonance regime. These researches provide theoretical references for experimental measurements.
Published Version
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