Theoretical aspects of femtosecond double-pump single-molecule spectroscopy. I. Weak-field regime
文献情報
Elisa Palacino-González, Maxim F. Gelin, Wolfgang Domcke
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.
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