Dipartimento di Fisica, Politecnico di Milano, Piazza L. da Vinci 32, 20133 Milano, Italy.
Phys Chem Chem Phys. 2010 Jul 28;12(28):7917-23. doi: 10.1039/c000505c. Epub 2010 May 27.
By applying femtosecond pump-probe spectroscopy to a substituted quinquethiophene molecule in solution, we observe in the time domain the coherent torsional dynamics that drives planarization of the excited state. Our interpretation is based on numerical modeling of the ground and excited state potential energy surfaces and simulation of wavepacket dynamics, which reveals two symmetric excited state deactivation pathways per oscillation period. We use the acquired knowledge on torsional dynamics to coherently control the excited state population with a pump-dump scheme, exploiting the non-stationary Franck-Condon overlap between ground and excited states.
通过飞秒泵浦探测光谱法研究溶液中取代的五噻吩分子,我们在时域中观察到了驱动激发态平面化的相干扭转动力学。我们的解释基于对基态和激发态势能面的数值建模和波包动力学的模拟,该模拟揭示了每个振荡周期有两条对称的激发态失活途径。我们利用扭转动力学方面的知识,通过泵浦-排空方案来实现对激发态布居的相干控制,利用基态和激发态之间的非定常 Franck-Condon 重叠。