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Understanding Primary Charge Separation in the Heliobacterial Reaction Center

Cite this: J. Phys. Chem. Lett. 2023, 14, 13, 3092–3102
Publication Date (Web):March 23, 2023
https://doi.org/10.1021/acs.jpclett.3c00377
Copyright © 2023 The Authors. Published by American Chemical Society

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    Abstract

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    The homodimeric reaction center of heliobacteria retains features of the ancestral reaction center and can thus provide insights into the evolution of photosynthesis. Primary charge separation is expected to proceed in a two-step mechanism along either of the two reaction center branches. We reveal the first charge-separation step from first-principles calculations based on time-dependent density functional theory with an optimally tuned range-separated hybrid and ab initio Born–Oppenheimer molecular dynamics: the electron is most likely localized on the electron transfer cofactor 3 (EC3, OH-chlorophyll a), and the hole on the adjacent EC2. Including substantial parts of the surrounding protein environment into the calculations shows that a distinct structural mechanism is decisive for the relative energetic positioning of the electronic excitations: specific charged amino acids in the vicinity of EC3 lower the energy of charge-transfer excitations and thus facilitate efficient charge separation. These results are discussed considering recent experimental insights.

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    • Description of the different structural units; details on the TDDFT excitation spectra, and the BOMD analysis; automated protocol for the analysis of excitation spectra (PDF)

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    Cited By

    This article is cited by 1 publications.

    1. Akihiro Kimura, Hirotaka Kitoh-Nishioka, Toru Kondo, Hirozo Oh-oka, Shigeru Itoh, Chihiro Azai. Experimental and Theoretical Mutation of Exciton States on the Smallest Type-I Photosynthetic Reaction Center Complex of a Green Sulfur Bacterium Chlorobaclum tepidum. The Journal of Physical Chemistry B 2024, 128 (3) , 731-743. https://doi.org/10.1021/acs.jpcb.3c07424