TY - JOUR
T1 - Nonadiabatic one-electron transfer mechanism for the O–O bond formation in the oxygen-evolving complex of photosystem II
AU - Shoji, Mitsuo
AU - Isobe, Hiroshi
AU - Shigeta, Yasuteru
AU - Nakajima, Takahito
AU - Yamaguchi, Kizashi
N1 - Funding Information:
This research was supported by JSPS KAKENHI Grant Numbers JP24000018 and JP17H04866 . Numerical calculations have been carried out under the supports of (1) HPCI system research project (Project ID: hp160169 ) using the computational resource of the center for computational sciences (CCS), University of Tsukuba, (2) “Interdisciplinary Computational Science Program” at CCS, (3) the research center for computational Sciences, Okazaki, Japan, and (4) HPCI system research projects (Project ID: hp150128 and hp160170) using the computational resources of the K computer provided by the RIKEN Advanced Institute for Computational Science (AICS).
PY - 2018/4/16
Y1 - 2018/4/16
N2 - The reaction mechanism of the O2 formation in the S4 state of the oxygen-evolving complex of photosystem II was clarified at the quantum mechanics/molecular mechanics (QM/MM) level. After the Yz (Y161) oxidation and the following proton transfer in the S3 state, five reaction steps are required to produce the molecular dioxygen. The highest barrier step is the first proton transfer reaction (0 → 1). The following reactions involving electron transfers were precisely analyzed in terms of their energies, structures and spin densities. We found that the one-electron transfer from the Mn4Ca cluster to Y161 triggers the O–O sigma bond formation.
AB - The reaction mechanism of the O2 formation in the S4 state of the oxygen-evolving complex of photosystem II was clarified at the quantum mechanics/molecular mechanics (QM/MM) level. After the Yz (Y161) oxidation and the following proton transfer in the S3 state, five reaction steps are required to produce the molecular dioxygen. The highest barrier step is the first proton transfer reaction (0 → 1). The following reactions involving electron transfers were precisely analyzed in terms of their energies, structures and spin densities. We found that the one-electron transfer from the Mn4Ca cluster to Y161 triggers the O–O sigma bond formation.
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U2 - 10.1016/j.cplett.2018.02.056
DO - 10.1016/j.cplett.2018.02.056
M3 - Article
AN - SCOPUS:85044000183
SN - 0009-2614
VL - 698
SP - 138
EP - 146
JO - Chemical Physics Letters
JF - Chemical Physics Letters
ER -