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Long-range coherent energy transport in Photosystem II

机译:光系统II中的远程相干能量传输

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摘要

We simulate the long-range inter-complex electronic energy transfer inPhotosystem II -- from the antenna complex, via a core complex, to the reactioncenter -- using a non-Markovian (ZOFE) quantum master equation description thatallows us to quantify the electronic coherence involved in the energy transfer.We identify the pathways of the energy transfer in the network of coupledchromophores, using a description based on excitation probability currents. Weinvestigate how the energy transfer depends on the initial excitation --localized, coherent initial excitation versus delocalized, incoherent initialexcitation -- and find that the energy transfer is remarkably robust withrespect to such strong variations of the initial condition. To explore theimportance of vibrationally enhanced transfer and to address the question ofoptimization in the system parameters, we vary the strength of the couplingbetween the electronic and the vibrational degrees of freedom. We find that theoriginal parameters lie in a (broad) region that enables optimal transferefficiency, and that the energy transfer appears to be very robust with respectto variations in the vibronic coupling. Nevertheless, vibrationally enhancedtransfer appears to be crucial to obtain a high transfer efficiency. We compareour quantum simulation to a "classical" rate equation based on amodified-Redfield/generalized-F\"orster description that was previously used tosimulate energy transfer dynamics in the entire Photosystem II complex, andfind very good agreement between quantum and rate-equation simulation of theoverall energy transfer dynamics.
机译:我们使用非马尔可夫(ZOFE)量子主方程描述来模拟Photosystem II中从天线复合物到核中心再到反应中心的远距离复合物电子能量转移,这使我们能够量化电子相干性我们使用基于激发概率电流的描述来识别耦合发色团网络中能量转移的途径。我们研究了能量转移如何取决于初始激发-局部,相干的初始激发与离域,非相干的初始激发-并发现,对于初始条件的这种强烈变化,能量转移具有显着的鲁棒性。为了探讨振动增强传递的重要性并解决系统参数优化的问题,我们改变了电子自由度和振动自由度之间的耦合强度。我们发现,原始参数位于能够实现最佳传递效率的(较宽的)区域内,并且能量传递对于振动耦合的变化似乎非常稳健。但是,振动增强的传输对于获得高传输效率似乎至关重要。我们将量子模拟与基于修正的Redfield / generalized-F'orster描述的“经典”速率方程进行比较,该方程先前用于模拟整个Photosystem II复合体中的能量传递动力学,并在量子和速率方程模拟之间找到了很好的一致性能量转移动力学

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