Mujica-Martinez C A, Nalbach P, Thorwart M
I. Institut für Theoretische Physik, Universität Hamburg, Jungiusstraße 9, 20355 Hamburg, Germany.
Phys Rev E Stat Nonlin Soft Matter Phys. 2013 Dec;88(6):062719. doi: 10.1103/PhysRevE.88.062719. Epub 2013 Dec 19.
The excitation energy transfer dynamics in the Fenna-Matthews-Olson complex is quantified in terms of a non-Markovianity measure based on the time evolution of the trace distance of two quantum states. We use a system description derived from experiments and different environmental fluctuation spectral functions, which are obtained either from experimental data or from molecular dynamics simulations. These exhibit, in all cases, a nontrivial structure with several peaks attributed to vibrational modes of the pigment-protein complex. Such a structured environmental spectrum can, in principle, give rise to strong non-Markovian effects. We present numerically exact real-time path-integral calculations for the transfer dynamics and find, in all cases, a monotonic decrease of the trace distance with increasing time which renders a Markovian description valid.
基于两个量子态的迹距离随时间的演化,通过非马尔可夫性度量对费纳 - 马修斯 - 奥尔森复合物中的激发能量转移动力学进行了量化。我们使用从实验和不同环境涨落谱函数导出的系统描述,这些谱函数要么从实验数据中获得,要么从分子动力学模拟中获得。在所有情况下,这些谱函数都呈现出具有几个归因于色素 - 蛋白质复合物振动模式的峰的非平凡结构。原则上,这样的结构化环境谱会产生强烈的非马尔可夫效应。我们给出了转移动力学的数值精确实时路径积分计算结果,并且在所有情况下都发现,随着时间的增加,迹距离单调减小,这使得马尔可夫描述有效。