期刊
NATURE COMMUNICATIONS
卷 12, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-021-23060-9
关键词
-
资金
- Office of Basic Energy Sciences
- US Department of Energy [DE-SC0016384]
- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, of the US Department of Energy [DE-SC0010575]
- Lithuanian Science Council [S-MIP-20-47]
- U.S. Department of Energy (DOE) [DE-SC0016384] Funding Source: U.S. Department of Energy (DOE)
Researchers investigated the heliobacterial reaction center using spectroscopic studies, identifying the primary pathway and mechanism of charge separation, and confirming that charge separation occurs through a single pathway with a specific electron acceptor.
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. The primary energy conversion step in photosynthesis, charge separation, takes place in the reaction center. Here the authors investigate the heliobacterial reaction center using multispectral two-dimensional electronic spectroscopy, identifying the primary electron acceptor and revealing the charge separation mechanism.
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