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Manuscript-HbRC-submitted-Nov13-YS.pdf (1.19 MB)

Excitonic Structure and Charge Separation in the Heliobacterial Reaction Center Probed by Multispectral Multidimensional Spectroscopy

preprint
revised on 28.01.2021, 21:59 and posted on 29.01.2021, 13:20 by Yin Song, Riley Sechrist, Hoang Huy Nguyen, William Johnson, Darius Abramavičius, Kevin Redding, Jennifer P. Ogilvie

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 A0 chlorophyll a pigment is the primary electron acceptor. In addition, we find strong delocalization of the initial excited state and 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.

History

Email Address of Submitting Author

songyi@umich.edu

Institution

University of Michigan

Country

US

ORCID For Submitting Author

0000-0001-8978-2958

Declaration of Conflict of Interest

no conflict of interest

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ChemRxiv

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