Vibronic contributions to resonant NLO responses: two-photon absorption in push-pull chromophores

Physics – Chemical Physics

Scientific paper

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10 pages including 3 figures

Scientific paper

10.1016/S0009-2614(01)00994-0

Two-photon absorption (TPA) spectra of push-pull chromophores are described in terms of a two-state model accounting for electron-vibration coupling. Vibrations have two main effects in TPA spectra. The most obvious one is the appearance of a vibrational structure in the spectrum; in this respect we find large Herzberg-Teller contributions. The second effect was not recognized so far: vibrational states contribute a new channel to TPA process, that shows up with a blue-shift and a distortion of the spectrum. Vibrational-channel contributions to other NLO responses are shortly discussed.

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