Minerals and Materials Science and Technology, Mawson Institute, Division of ITEE, University of South Australia, Adelaide, South Australia 5095, Australia.
J Chem Phys. 2012 Feb 14;136(6):065104. doi: 10.1063/1.3684654.
The non-Hermitian quantum dynamics of excitonic energy transfer in photosynthetic systems is investigated using a dissipative two-level dimer model. The approach is based on Green's function formalism which permits consideration of decoherence and intersite transfer processes on comparable terms. The results indicate a combination of coherent and incoherent behavior at higher temperatures with the possibility of exceptional points occurring at the coherent-incoherent crossover regime at critical temperatures. When each dimer site is coupled equally to the environmental sources of dissipation, the excitonic wavepacket evolves with time with a coherent component, which can be attributed to the indistinguishability of the sources of dissipation. The time evolution characteristics of the B850 Bchls dimer system is analysed using typical parameter estimates in photosynthetic systems, and the quantum brachistochrone passage times are obtained for a range of parameters.
本文采用耗散双能级二聚体模型研究了光合系统中激子能量转移的非厄米量子动力学。该方法基于格林函数形式主义,可以在可比条件下考虑退相干和局域转移过程。结果表明,在较高温度下存在相干和非相干行为的组合,在临界温度的相干-非相干交叉区域可能出现异常点。当每个二聚体位点与环境耗散源相等耦合时,激子波包随时间演化具有相干分量,这可以归因于耗散源的不可区分性。使用光合系统中的典型参数估计分析了 B850 Bchls 二聚体系统的时间演化特征,并获得了一系列参数下的量子最短时间。