Theoretical and computational investigations of geometrical, electronic and spin structures of the CaMn 4 O X (X = 5, 6) cluster in the Kok cycle S i (i = 0–3) of oxygen evolving complex of photosystem II

Kizashi Yamaguchi, Shusuke Yamanaka, Hiroshi Isobe, Mitsuo Shoji, Kouichi Miyagawa, Takahito Nakajima, Takashi Kawakami, Mitsutaka Okumura

Research output: Contribution to journal › Article

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Abstract

The optimized geometries of the CaMn 4 O X (X = 5, 6) cluster in the oxygen evolving complex (OEC) of photosystem II (PSII) by large-scale quantum mechanics (QM) and molecular mechanics (MM) calculations are compared with recent serial femtosecond crystallography (SFX) results for the S i (i = 0–3) states. The valence states of four Mn ions by the QM/MM calculations are also examined in relation to the experimental results by the X-ray emission spectroscopy (XES) for the S i intermediates. Geometrical and valence structures of right-opened Mn-hydroxide, Mn-oxo and Mn-peroxide intermediates in the S 3 state are investigated in detail in relation to recent SFX and XES experiments for the S 3 state. Interplay between theory and experiment indicates that the Mn-oxo intermediate is a new possible candidate for the S 3 state. Implications of the computational results are discussed in relation to possible mechanisms of the oxygenoxygen bond formation for water oxidation in OEC of PSII.

Original languageEnglish
JournalPhysiologia Plantarum
DOIs
Publication statusPublished - Jan 1 2019

Fingerprint

oxygen evolving complex
Photosystem II Protein Complex
Mechanics
mechanics
photosystem II
electronics
spectroscopy
X-radiation
crystallography
X-Ray Emission Spectrometry
Oxygen
hydroxides
peroxides
oxidation
ions
Crystallography
Peroxides
water
Ions
quantum mechanics

ASJC Scopus subject areas

  • Physiology
  • Genetics
  • Plant Science
  • Cell Biology

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Theoretical and computational investigations of geometrical, electronic and spin structures of the CaMn 4 O X (X = 5, 6) cluster in the Kok cycle S i (i = 0–3) of oxygen evolving complex of photosystem II . / Yamaguchi, Kizashi; Yamanaka, Shusuke; Isobe, Hiroshi; Shoji, Mitsuo; Miyagawa, Kouichi; Nakajima, Takahito; Kawakami, Takashi; Okumura, Mitsutaka.

In: Physiologia Plantarum, 01.01.2019.

Research output: Contribution to journal › Article

Yamaguchi, K, Yamanaka, S, Isobe, H, Shoji, M, Miyagawa, K, Nakajima, T, Kawakami, T & Okumura, M 2019, ' Theoretical and computational investigations of geometrical, electronic and spin structures of the CaMn 4 O X (X = 5, 6) cluster in the Kok cycle S i (i = 0–3) of oxygen evolving complex of photosystem II ', Physiologia Plantarum. https://doi.org/10.1111/ppl.12960
Yamaguchi K, Yamanaka S, Isobe H, Shoji M, Miyagawa K, Nakajima T et al. Theoretical and computational investigations of geometrical, electronic and spin structures of the CaMn 4 O X (X = 5, 6) cluster in the Kok cycle S i (i = 0–3) of oxygen evolving complex of photosystem II Physiologia Plantarum. 2019 Jan 1. https://doi.org/10.1111/ppl.12960
Yamaguchi, Kizashi ; Yamanaka, Shusuke ; Isobe, Hiroshi ; Shoji, Mitsuo ; Miyagawa, Kouichi ; Nakajima, Takahito ; Kawakami, Takashi ; Okumura, Mitsutaka. / Theoretical and computational investigations of geometrical, electronic and spin structures of the CaMn 4 O X (X = 5, 6) cluster in the Kok cycle S i (i = 0–3) of oxygen evolving complex of photosystem II In: Physiologia Plantarum. 2019.
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abstract = "The optimized geometries of the CaMn 4 O X (X = 5, 6) cluster in the oxygen evolving complex (OEC) of photosystem II (PSII) by large-scale quantum mechanics (QM) and molecular mechanics (MM) calculations are compared with recent serial femtosecond crystallography (SFX) results for the S i (i = 0–3) states. The valence states of four Mn ions by the QM/MM calculations are also examined in relation to the experimental results by the X-ray emission spectroscopy (XES) for the S i intermediates. Geometrical and valence structures of right-opened Mn-hydroxide, Mn-oxo and Mn-peroxide intermediates in the S 3 state are investigated in detail in relation to recent SFX and XES experiments for the S 3 state. Interplay between theory and experiment indicates that the Mn-oxo intermediate is a new possible candidate for the S 3 state. Implications of the computational results are discussed in relation to possible mechanisms of the oxygenoxygen bond formation for water oxidation in OEC of PSII.",
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AU - Miyagawa, Kouichi

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AU - Kawakami, Takashi

AU - Okumura, Mitsutaka

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