Laboratory of Physical Chemistry, ETH Zürich, 8093 Zürich, Switzerland.
J Phys Chem Lett. 2022 Apr 21;13(15):3392-3399. doi: 10.1021/acs.jpclett.2c00538. Epub 2022 Apr 11.
Photosynthetic organisms are known to use a mechanism of vibrationally assisted exciton energy transfer to efficiently harvest energy from light. The importance of quantum effects in this mechanism is a long-standing topic of debate, which has traditionally focused on the role of excitonic coherences. Here, we address another recent claim: that the efficient energy transfer in the Fenna-Matthews-Olson complex relies on nuclear quantum uncertainty and would not function if the vibrations were classical. We present a counter-example to this claim, showing by trajectory-based simulations that a description in terms of quantum electrons and classical nuclei is indeed sufficient to describe the funneling of energy to the reaction center. We analyze and compare these findings to previous classical-nuclear approximations that predicted the absence of an energy funnel and conclude that the key difference and the reason for the discrepancy is the ability of the trajectories to properly account for Newton's third law.
已知光合生物利用振动辅助激子能量转移的机制来有效地从光中获取能量。在这个机制中,量子效应的重要性是一个长期存在的争论话题,传统上一直集中在激子相干的作用上。在这里,我们讨论另一个最近的观点:即 Fenna-Matthews-Olson 复合物中的有效能量转移依赖于核量子不确定性,如果振动是经典的,那么它将无法发挥作用。我们提出了一个对此观点的反例,通过基于轨迹的模拟表明,基于量子电子和经典原子核的描述确实足以描述能量向反应中心的传递。我们分析并比较了这些发现与之前预测不存在能量漏斗的经典-原子核近似,得出的结论是关键的区别和差异的原因是轨迹能够正确地解释牛顿第三定律。