光合反应中心
离域电子
化学物理
光谱学
电子结构
电荷(物理)
细菌叶绿素
多光谱图像
密度泛函理论
化学
材料科学
光合作用
光化学
计算化学
物理
计算机科学
电子转移
量子力学
有机化学
生物化学
计算机视觉
作者
Yin Song,Riley Sechrist,Hoang Huy Nguyen,William A. Johnson,Darius Abramavičius,Kevin Redding,Jennifer P. Ogilvie
标识
DOI:10.1038/s41467-021-23060-9
摘要
Abstract Photochemical reaction centers are the engines that drive photosynthesis. The reaction center from heliobacteria (HbRC) has been proposed to most closely resemble the common ancestor of photosynthetic reaction centers, motivating a detailed understanding of its structure-function relationship. The recent elucidation of the HbRC crystal structure motivates advanced spectroscopic studies of its excitonic structure and charge separation mechanism. We perform multispectral two-dimensional electronic spectroscopy of the HbRC and corresponding numerical simulations, resolving the electronic structure and testing and refining recent excitonic models. Through extensive examination of the kinetic data by lifetime density analysis and global target analysis, we reveal that charge separation proceeds via a single pathway in which the distinct A 0 chlorophyll a pigment is the primary electron acceptor. In addition, we find strong delocalization of the charge separation intermediate. Our findings have general implications for the understanding of photosynthetic charge separation mechanisms, and how they might be tuned to achieve different functional goals.
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