TY - JOUR
T1 - Elucidation of the entire Kok cycle for photosynthetic water oxidation by the large-scale quantum mechanics/molecular mechanics calculations
T2 - Comparison with the experimental results by the recent serial femtosecond crystallography
AU - Shoji, Mitsuo
AU - Isobe, Hiroshi
AU - Shen, Jian Ren
AU - Suga, Michihiro
AU - Akita, Fusamichi
AU - Miyagawa, Koichi
AU - Shigeta, Yasuteru
AU - Yamaguchi, Kizashi
N1 - Funding Information:
One of the authors (K. Y) thank Prof. N. Kamiya, Dr. K. Kawakami and Dr. Umena for helpful discussions on the experimental uncertainty of the Mn
Funding Information:
One of the authors (K. Y) thank Prof. N. Kamiya, Dr. K. Kawakami and Dr. Umena for helpful discussions on the experimental uncertainty of the Mn O O 4 (5) and O (5) (6) distances of the CaMn 4 O x ( x = 5, 6) clusters by the XRD [4,5] and SFX-XFEL [10–12] experiments on OEC of PSII. K. Y. also thanks Dr. J. Kern for kind discussions on the possible S 3 intermediate in the Kok cycle. 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) the “Interdisciplinary Computational Science Program” at the Center for Computational Sciences (CCS) in University of Tsukuba, (2) Research Center for Computational Science, Okazaki, Japan, and (3) HPCI systems (Project ID: hp180163 and hp180154).
Publisher Copyright:
© 2019 Elsevier B.V.
PY - 2019/9
Y1 - 2019/9
N2 - The fully optimized geometrical structures of the CaMn4Ox (x = 5, 6) clusters in the Si (i = 0–3) states of the Kok cycle of photosynthetic water oxidation by the large-scale quantum mechanics/molecular mechanics (QM/MM) calculations were compared to recent experimental results based on serial femtosecond crystallography (SFX). The Mn–Mn and Ca–Mn distances obtained by the QM/MM calculations were found to be totally comparable to the SFX experiments, elucidating the entire Kok cycle involving the S4 transition state during the O–O bond formation for water oxidation in the oxygen evolving complex (OEC) of photosystem II (PSII).
AB - The fully optimized geometrical structures of the CaMn4Ox (x = 5, 6) clusters in the Si (i = 0–3) states of the Kok cycle of photosynthetic water oxidation by the large-scale quantum mechanics/molecular mechanics (QM/MM) calculations were compared to recent experimental results based on serial femtosecond crystallography (SFX). The Mn–Mn and Ca–Mn distances obtained by the QM/MM calculations were found to be totally comparable to the SFX experiments, elucidating the entire Kok cycle involving the S4 transition state during the O–O bond formation for water oxidation in the oxygen evolving complex (OEC) of photosystem II (PSII).
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U2 - 10.1016/j.cplett.2019.06.026
DO - 10.1016/j.cplett.2019.06.026
M3 - Article
AN - SCOPUS:85067401446
VL - 730
SP - 416
EP - 425
JO - Chemical Physics Letters
JF - Chemical Physics Letters
SN - 0009-2614
ER -