Signatures of three-exciton correlations in the coherent and incoherent nonlinear optical response of photosynthetic complexes

Signatures of three-exciton correlations in the coherent and incoherent nonlinear optical response of photosynthetic complexes
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光合复合物相干和非相干非线性光学响应中三激子相关性的特征

DOI:
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发表时间:
2010
期刊:
影响因子:
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通讯作者:
S. Mukamel
S. Mukamel
中科院分区:
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文献类型:
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作者:
Li;D. Abramavičius;S. Mukamel

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我们模拟研究了Fenna-Matthews-Olson(FMO)捕光光合作用复合体三阶非线性响应中的布居和相干弛豫动力学。引入了三激子关联,并计算了与声子浴耦合的六点弛豫超算符的二阶。当三激子变量因式分解时,三激子关联的动力学产生了新的峰,这些峰是不存在的或弱得多的。在最近的一项实验中观察到了这些特征(恩格尔·G·S等人,2007年,《自然》杂志,446782-6)。
We present a simulation study of population and coherence relaxation dynamics in the third-order nonlinear responses of the Fenna–Matthews–Olson (FMO) light-harvesting photosynthetic complex. Three-exciton correlations have been incorporated and the relevant six-point relaxation superoperator is calculated to second order in coupling to a phonon bath. The dynamics of three-exciton correlations induce new peaks that are absent or much weaker when the three-exciton variables are factorized. Such features were observed in a recent experiment (Engel G S et al 2007 Nature 446 782–6).