振动子对NLO共振响应的贡献：推挽发色团中的双光子吸收
Vibronic contributions to resonant NLO responses: two-photon absorption in push-pull chromophores
摘要：
用考虑电子振动耦合的双态模型描述了推挽式发色团的双光子吸收光谱。振动在TPA光谱中有两个主要影响。最明显的一个是在光谱中出现的振动结构，在这方面，我们发现大赫兹伯格-泰勒贡献。第二个效应是迄今为止尚未认识到的：振动态为TPA过程提供了一个新的通道，表现为光谱的蓝移和畸变。振动通道的贡献，其他非线性振荡响应进行了简短的讨论。
英文摘要：
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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