TY - JOUR
T1 - An oxyl/oxo mechanism for oxygen-oxygen coupling in PSII revealed by an x-ray free-electron laser
AU - Suga, Michihiro
AU - Akita, Fusamichi
AU - Yamashita, Keitaro
AU - Nakajima, Yoshiki
AU - Ueno, Go
AU - Li, Hongjie
AU - Yamane, Takahiro
AU - Hirata, Kunio
AU - Umena, Yasufumi
AU - Yonekura, Shinichiro
AU - Yu, Long Jiang
AU - Murakami, Hironori
AU - Nomura, Takashi
AU - Kimura, Tetsunari
AU - Kubo, Minoru
AU - Baba, Seiki
AU - Kumasaka, Takashi
AU - Tono, Kensuke
AU - Yabashi, Makina
AU - Isobe, Hiroshi
AU - Yamaguchi, Kizashi
AU - Yamamoto, Masaki
AU - Ago, Hideo
AU - Shen, Jian Ren
N1 - Funding Information:
The x-ray free electron laser experiments were performed at SACLA with the approval of the Japan Synchrotron Radiation Research Institute (JASRI) (proposal nos. 2016A8051, 2016B8070, 2017A8040, 2017B8015, 2017B8028, 2018A8009, and 2018A8010), and we thank the staff at SACLA for their help. The best condition for diffraction data collection was determined at beamlines 41XU and 44XU in SPring-8 (proposal nos. 2016A2542, 2016A6621, 2016B2542, 2016B6621, 2017A2535, 2017A6724, 2017B2535, 2017B6724, 2018A2530, 2018A6822, 2018B2530, and 2018B6822). his research was supported by the Platform Project for Supporting Drug Discovery and Life Science Research [Basis for Supporting Innovative Drug Discovery and Life Science Research (BINDS)] from AMED under grant JP18am0101070. This research was also supported by KAKENHI grants JP16H06162, JP16H06296, and JP17H05884 (M.S.); JP17H06434 (J.-R.S.); and JP16K21181 (F.A.). Support was also provided by JST, PREST grants JPMJPR18G8 (M.S.) and JPMJPR16P1 (F.A.), and RIKEN Pioneering Project ?Dynamic Structural Biology? to M.K. and M.Yam.
Publisher Copyright:
Copyright © 2019 The Authors,
PY - 2019/10/18
Y1 - 2019/10/18
N2 - Photosynthetic water oxidation is catalyzed by the Mn4CaO5 cluster of photosystem II (PSII) with linear progression through five S-state intermediates (S0 to S4). To reveal the mechanism of water oxidation, we analyzed structures of PSII in the S1, S2, and S3 states by x-ray free-electron laser serial crystallography. No insertion of water was found in S2, but flipping of D1 Glu189 upon transition to S3 leads to the opening of a water channel and provides a space for incorporation of an additional oxygen ligand, resulting in an open cubane Mn4CaO6 cluster with an oxyl/oxo bridge. Structural changes of PSII between the different S states reve cooperative action of substrate water access, proton release, and dioxygen formation in photosynthetic water oxidation.
AB - Photosynthetic water oxidation is catalyzed by the Mn4CaO5 cluster of photosystem II (PSII) with linear progression through five S-state intermediates (S0 to S4). To reveal the mechanism of water oxidation, we analyzed structures of PSII in the S1, S2, and S3 states by x-ray free-electron laser serial crystallography. No insertion of water was found in S2, but flipping of D1 Glu189 upon transition to S3 leads to the opening of a water channel and provides a space for incorporation of an additional oxygen ligand, resulting in an open cubane Mn4CaO6 cluster with an oxyl/oxo bridge. Structural changes of PSII between the different S states reve cooperative action of substrate water access, proton release, and dioxygen formation in photosynthetic water oxidation.
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U2 - 10.1126/science.aax6998
DO - 10.1126/science.aax6998
M3 - Article
C2 - 31624207
AN - SCOPUS:85073603536
VL - 366
SP - 334
EP - 338
JO - Science
JF - Science
SN - 0036-8075
IS - 6463
ER -