Concerted bond switching mechanism coupled with one-electron transfer for the oxygen-oxygen bond formation in the oxygen-evolving complex of photosystem II

Mitsuo Shoji; Hiroshi Isobe; Kizashi Yamaguchi

doi:10.1016/j.cplett.2018.10.041

Concerted bond switching mechanism coupled with one-electron transfer for the oxygen-oxygen bond formation in the oxygen-evolving complex of photosystem II

Mitsuo Shoji, Hiroshi Isobe, Kizashi Yamaguchi

Research Institute for Interdisciplinary Science

Research output: Contribution to journal › Article › peer-review

5 Citations (Scopus)

Abstract

We here precisely analyzed the electronic structures during the oxygen-oxygen (O-O) bond formation of the oxygen-evolving complex (OEC) in photosystem II (PSII) based on the quantum mechanics/molecular mechanics (QM/MM) calculations. Changes in the spin density and the chemical indices derived from the natural orbitals suggested that the O₍₅₎-O₍₆₎ bond formation proceeds with a concerted bond breaking of the Mn₄-O₍₅₎ coupled with the through-bond one-electron transfer from the O₍₆₎ site to the Mn₄ site (Mn₄(IV) → Mn₄(III)). This mechanism can be best described as a Concerted Bond Switching (CBS) mechanism, which is a non-radical reaction of the O₍₅₎-O₍₆₎ bond formation.

Original language	English
Pages (from-to)	219-226
Number of pages	8
Journal	Chemical Physics Letters
Volume	714
DOIs	https://doi.org/10.1016/j.cplett.2018.10.041
Publication status	Published - Jan 16 2019

ASJC Scopus subject areas

Physics and Astronomy(all)
Physical and Theoretical Chemistry

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title = "Concerted bond switching mechanism coupled with one-electron transfer for the oxygen-oxygen bond formation in the oxygen-evolving complex of photosystem II",

abstract = "We here precisely analyzed the electronic structures during the oxygen-oxygen (O-O) bond formation of the oxygen-evolving complex (OEC) in photosystem II (PSII) based on the quantum mechanics/molecular mechanics (QM/MM) calculations. Changes in the spin density and the chemical indices derived from the natural orbitals suggested that the O(5)-O(6) bond formation proceeds with a concerted bond breaking of the Mn4-O(5) coupled with the through-bond one-electron transfer from the O(6) site to the Mn4 site (Mn4(IV) → Mn4(III)). This mechanism can be best described as a Concerted Bond Switching (CBS) mechanism, which is a non-radical reaction of the O(5)-O(6) bond formation.",

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T1 - Concerted bond switching mechanism coupled with one-electron transfer for the oxygen-oxygen bond formation in the oxygen-evolving complex of photosystem II

AU - Shoji, Mitsuo

AU - Isobe, Hiroshi

AU - Yamaguchi, Kizashi

PY - 2019/1/16

Y1 - 2019/1/16

N2 - We here precisely analyzed the electronic structures during the oxygen-oxygen (O-O) bond formation of the oxygen-evolving complex (OEC) in photosystem II (PSII) based on the quantum mechanics/molecular mechanics (QM/MM) calculations. Changes in the spin density and the chemical indices derived from the natural orbitals suggested that the O(5)-O(6) bond formation proceeds with a concerted bond breaking of the Mn4-O(5) coupled with the through-bond one-electron transfer from the O(6) site to the Mn4 site (Mn4(IV) → Mn4(III)). This mechanism can be best described as a Concerted Bond Switching (CBS) mechanism, which is a non-radical reaction of the O(5)-O(6) bond formation.

AB - We here precisely analyzed the electronic structures during the oxygen-oxygen (O-O) bond formation of the oxygen-evolving complex (OEC) in photosystem II (PSII) based on the quantum mechanics/molecular mechanics (QM/MM) calculations. Changes in the spin density and the chemical indices derived from the natural orbitals suggested that the O(5)-O(6) bond formation proceeds with a concerted bond breaking of the Mn4-O(5) coupled with the through-bond one-electron transfer from the O(6) site to the Mn4 site (Mn4(IV) → Mn4(III)). This mechanism can be best described as a Concerted Bond Switching (CBS) mechanism, which is a non-radical reaction of the O(5)-O(6) bond formation.

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