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Internal Conversion Process of Chlorophyll a in Solvents in Femtosecond Pump-Probe Laser Fields
Kai Niu,Li-qing Dong,Shu-lin Cong¤
Author NameAffiliationE-mail
Kai Niu Department of Physics, Dalian University of Technology, Dalian 116024, China  
Li-qing Dong Department of Physics, Dalian University of Technology, Dalian 116024, China  
Shu-lin Cong¤ Department of Physics, Dalian University of Technology, Dalian 116024, China shlcong@dlut.edu.cn 
Abstract:
The internal conversion (IC) processes of chlorophyll a (chl-a) in solvents are studied based on the reduced density matrix theory. The IC times can be obtained by simulating the experimental fluorescence depletion spectra (FDS). The calculated IC times of chl-a in ethyl acetate, tetrahydrofuran and dimethyl formamide are 141, 147, and 241 fs, respectively. The oscillation feature of the FDS results from the forward and backward transfer of the population between coupled electronic states. The effects of diabatic coupling between two electronic states on the IC time and the FDS are described. The influence of molecule-reservoir coupling on the IC time is also investigated.
Key words:  Fluorescence depletion spectrum, Internal conversion, Reduced density matrix
FundProject:国家自然科学基金
Internal Conversion Process of Chlorophyll a in Solvents in Femtosecond Pump-Probe Laser Fields
牛凯,董莉清,丛书林¤
摘要:
采用约化密度矩阵理论研究了溶液中叶绿素a分子的内转换过程. 内转换时间可以通过模拟实验荧光亏蚀光谱得到. 计算得到的叶绿素a分子在乙酸乙酯、四氢呋喃和二甲基甲酰胺溶剂中的内转换时间分别是141、147和241 fs. 理论分析表明:荧光亏蚀光谱曲线的振荡行为主要是由分子布居在耦合势能面间的振荡引起的. 分析了两个电子态之间非绝热耦合对内转换时间及荧光亏蚀光谱的影响,还讨论了叶绿素a分子与溶液耦合作用对内转换时间的影响.
关键词:  荧光亏蚀光谱,内转换,约化密度矩阵
DOI:10.1088/1674-0068/21/03/211-216
分类号: