论文标题

从自由能结构中获得的光合作用转移的见解:连贯的运输,不连贯的跳跃和振动援助重新审视

Insights into photosynthetic energy transfer gained from free-energy structure: Coherent transport, incoherent hopping, and vibrational assistance revisited

论文作者

Ishizaki, Akihito, Fleming, Graham R.

论文摘要

在超舒用激光脉冲技术方面的巨大步伐已实现了复杂分子系统中动态过程的实时观察。具体而言,在光合系统的二维电子光谱中发现振荡瞬变刺激了许多理论研究,探讨了光收集过程的显着量子效率的可能物理机制。但是,所采用的理论已经达到了高度的复杂程度,并且变得复杂,因此很难深入了解微观过程和具有生物学意义的问题。在这项工作中,我们重新审视了所涉及的电子能量环境引起的波动的基本方面,并提出了一种简单的方法,可以通过漏斗型自由能景观中的直观图片来理解能量流。提供的能量转移的自由能描述表明,典型的光合系统几乎无障碍的制度运行。该方法还提供了有关考虑振动辅助必要性的相干和不相互能量传递和标准之间的区别的见解。

Giant strides in ultrashort laser pulse technology have enabled real-time observation of dynamical processes in complex molecular systems. Specifically, the discovery of oscillatory transients in the two-dimensional electronic spectra of photosynthetic systems stimulated a number of theoretical investigations exploring possible physical mechanisms of the remarkable quantum efficiency of light harvesting processes. However, the theories employed have reached a high degree of sophistication and have become complex, making it difficult to gain insights into microscopic processes and biologically significant questions. In this work, we revisit the elementary aspects of environment-induced fluctuations in the involved electronic energies and present a simple way to understand energy flow with the intuitive picture of relaxation in a funnel-type free-energy landscape. The presented free-energy description of energy transfer reveals that typical photosynthetic systems operate in an almost barrierless regime. The approach also provides insights into the distinction between coherent and incoherent energy transfer and criteria by which the necessity of the vibrational assistance is considered.

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