Determination of the Formation of Dark State via Depleted Spontaneous Emission in a Complex Solvated Molecule

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• 作者：Xunmin Guo ; Sufan Wang ; Andong Xia ; Hongmei Su
• 刊名：Journal of Physical Chemistry A
• 出版年：2007
• 出版时间：July 5, 2007
• 年：2007
• 卷：111
• 期：26
• 页码：5800 - 5805
• 全文大小：134K
• 年卷期：v.111,no.26(July 5, 2007)
• ISSN：1520-5215

文摘

We present a general two-color two-pulse femtosecond pump-dump approach to study the specific populationtransfer along the reaction coordinate through the higher vibrational energy levels of excited states of a complexsolvated molecule via the depleted spontaneous emission. The time-dependent fluorescence depletion providesthe correlated dynamical information between the monitored fluorescence state and the SEP "dumped" darkstates, and therefore allow us to obtain the dynamics of the formation of the dark states corresponding to theultrafast photoisomerization processes. The excited-state dynamics of LDS 751 have been investigated as afunction of solvent viscosity and solvent polarity, where a cooperative two-step isomerization process isclearly identified within LDS 751 upon excitation.