scholarly journals An oxyl/oxo mechanism for oxygen-oxygen coupling in PSII revealed by an x-ray free-electron laser

Science ◽  
2019 ◽  
Vol 366 (6463) ◽  
pp. 334-338 ◽  
Author(s):  
Michihiro Suga ◽  
Fusamichi Akita ◽  
Keitaro Yamashita ◽  
Yoshiki Nakajima ◽  
Go Ueno ◽  
...  

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 reveal cooperative action of substrate water access, proton release, and dioxygen formation in photosynthetic water oxidation.

2014 ◽  
Vol 369 (1647) ◽  
pp. 20130324 ◽  
Author(s):  
Rosalie Tran ◽  
Jan Kern ◽  
Johan Hattne ◽  
Sergey Koroidov ◽  
Julia Hellmich ◽  
...  

The structure of photosystem II and the catalytic intermediate states of the Mn 4 CaO 5 cluster involved in water oxidation have been studied intensively over the past several years. An understanding of the sequential chemistry of light absorption and the mechanism of water oxidation, however, requires a new approach beyond the conventional steady-state crystallography and X-ray spectroscopy at cryogenic temperatures. In this report, we present the preliminary progress using an X-ray free-electron laser to determine simultaneously the light-induced protein dynamics via crystallography and the local chemistry that occurs at the catalytic centre using X-ray spectroscopy under functional conditions at room temperature.


2011 ◽  
Vol 131 (2) ◽  
pp. 68-71
Author(s):  
Etsuo FUJIWARA ◽  
Eiichi ANAYAMA ◽  
Yuichiro KATSUTA ◽  
Toshiki IZUTANI ◽  
Daichi OKUHARA ◽  
...  

2014 ◽  
Vol 134 (12) ◽  
pp. 836-839
Author(s):  
Junichi INOUE ◽  
Yuji TANAKA ◽  
Yuki MATSUMOTO ◽  
Kensuke KANDA

Author(s):  
W. Singer ◽  
A. Brinkmann ◽  
R. Brinkmann ◽  
J. Iversen ◽  
A. Matheisen ◽  
...  

2020 ◽  
Vol 2 (4) ◽  
Author(s):  
Alexander Malyzhenkov ◽  
Yunieski P. Arbelo ◽  
Paolo Craievich ◽  
Philipp Dijkstal ◽  
Eugenio Ferrari ◽  
...  

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