Theoretical aspects of femtosecond double-pump single-molecule spectroscopy. I. Weak-field regime.
Theoretical aspects of femtosecond double-pump single-molecule spectroscopy. I. Weak-field regime.
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DOI：
10.1039/c7cp04809b
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发表时间：
2017
期刊：
影响因子：
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通讯作者：
Elisa Palacino-González;M. Gelin;W. Domcke
中科院分区：
文献类型：
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作者：
Elisa Palacino-González;M. Gelin;W. Domcke
本文从理论上描述了双泵浦飞秒单分子荧光探测信号。我们模拟这些信号在弱场制度的一个模型，模仿一个生色团的Franck-Condon活性振动模式。我们建立了几个签名，这些信号是弱场制度的特点。的签名包括淬火的振动跳动的电子退相和一个明显的倾斜的相位-时间分布在二维（2D）的地图。我们研究了环境诱导的电子退相和相关发色团参数（电子能量，取向，振动频率和相对位移的势能面）的缓慢调制如何影响信号。
We present a theoretical description of double-pump femtosecond single-molecule signals with fluorescence detection. We simulate these signals in the weak-field regime for a model mimicking a chromophore with a Franck-Condon-active vibrational mode. We establish several signatures of these signals which are characteristic for the weak-field regime. The signatures include the quenching of vibrational beatings by electronic dephasing and a pronounced tilt of the phase-time profiles in the two-dimensional (2D) maps. We study how environment-induced slow modulations of the electronic dephasing and relevant chromophore parameters (electronic energy, orientation, vibrational frequency and relative shift of the potential energy surfaces) affect the signals.