TY - JOUR
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
N1 - Funding Information:
This work has been supported by MEXT KAKENHI Grant Nos. JP18H05154 , JP18H05167 , JP17H06434 (MS, HI, KY) and JSPS KAKENHI Grant No. JP17H04866 . Numerical calculations were carried out under the supports from (1) Multidisciplinary Cooperative Research Program in Center for Computational Sciences (CCS), University of Tsukuba, Japan, (2) Research Center for Computational Science, Okazaki, Japan, and (3) HPCI system research projects (Project ID: hp180163 and hp180154).
Funding Information:
This work has been supported by MEXT KAKENHI Grant Nos. JP18H05154, JP18H05167, JP17H06434 (MS, HI, KY) and JSPS KAKENHI Grant No. JP17H04866. Numerical calculations were carried out under the supports from (1) Multidisciplinary Cooperative Research Program in Center for Computational Sciences (CCS), University of Tsukuba, Japan, (2) Research Center for Computational Science, Okazaki, Japan, and (3) HPCI system research projects (Project ID: hp180163 and hp180154).
Publisher Copyright:
© 2018 Elsevier B.V.
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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U2 - 10.1016/j.cplett.2018.10.041
DO - 10.1016/j.cplett.2018.10.041
M3 - Article
AN - SCOPUS:85056716472
VL - 714
SP - 219
EP - 226
JO - Chemical Physics Letters
JF - Chemical Physics Letters
SN - 0009-2614
ER -