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Verfasst von:Ibrahim, Mohamed [VerfasserIn]   i
 Fransson, Thomas [VerfasserIn]   i
 Chatterjee, Ruchira [VerfasserIn]   i
 Cheah, Mun Hon [VerfasserIn]   i
 Hussein, Rana [VerfasserIn]   i
 Lassalle, Louise [VerfasserIn]   i
 Sutherlin, Kyle D. [VerfasserIn]   i
 Young, Iris D. [VerfasserIn]   i
 Fuller, Franklin D. [VerfasserIn]   i
 Gul, Sheraz [VerfasserIn]   i
 Kim, In-Sik [VerfasserIn]   i
 Simon, Philipp S. [VerfasserIn]   i
 Lichtenberg, Casper de [VerfasserIn]   i
 Chernev, Petko [VerfasserIn]   i
 Bogacz, Isabel [VerfasserIn]   i
 Pham, Cindy C. [VerfasserIn]   i
 Orville, Allen M. [VerfasserIn]   i
 Saichek, Nicholas [VerfasserIn]   i
 Northen, Trent [VerfasserIn]   i
 Batyuk, Alexander [VerfasserIn]   i
 Carbajo, Sergio [VerfasserIn]   i
 Alonso-Mori, Roberto [VerfasserIn]   i
 Tono, Kensuke [VerfasserIn]   i
 Owada, Shigeki [VerfasserIn]   i
 Bhowmick, Asmit [VerfasserIn]   i
 Bolotovsky, Robert [VerfasserIn]   i
 Mendez, Derek [VerfasserIn]   i
 Moriarty, Nigel W. [VerfasserIn]   i
 Holton, James M. [VerfasserIn]   i
 Dobbek, Holger [VerfasserIn]   i
 Brewster, Aaron S. [VerfasserIn]   i
 Adams, Paul D. [VerfasserIn]   i
 Sauter, Nicholas K. [VerfasserIn]   i
 Bergmann, Uwe [VerfasserIn]   i
 Zouni, Athina [VerfasserIn]   i
 Messinger, Johannes [VerfasserIn]   i
 Kern, Jan [VerfasserIn]   i
 Yachandra, Vittal K. [VerfasserIn]   i
 Yano, Junko [VerfasserIn]   i
Titel:Untangling the sequence of events during the S2 → S3 transition in photosystem II and implications for the water oxidation mechanism
Verf.angabe:Mohamed Ibrahim, Thomas Fransson, Ruchira Chatterjee, Mun Hon Cheah, Rana Hussein, Louise Lassalle, Kyle D. Sutherlin, Iris D. Young, Franklin D. Fuller, Sheraz Gul, In-Sik Kim, Philipp S. Simon, Casper de Lichtenberg, Petko Chernev, Isabel Bogacz, Cindy C. Pham, Allen M. Orville, Nicholas Saichek, Trent Northen, Alexander Batyuk, Sergio Carbajo, Roberto Alonso-Mori, Kensuke Tono, Shigeki Owada, Asmit Bhowmick, Robert Bolotovsky, Derek Mendez, Nigel W. Moriarty, James M. Holton, Holger Dobbek, Aaron S. Brewster, Paul D. Adams, Nicholas K. Sauter, Uwe Bergmann, Athina Zouni, Johannes Messinger, Jan Kern, Vittal K. Yachandra, and Junko Yano
E-Jahr:2020
Jahr:9 June 2020
Umfang:12 S.
Fussnoten:Gesehen am 26.08.2020
Titel Quelle:Enthalten in: National Academy of Sciences (Washington, DC)Proceedings of the National Academy of Sciences of the United States of America
Ort Quelle:Washington, DC : National Acad. of Sciences, 1915
Jahr Quelle:2020
Band/Heft Quelle:117(2020), 23, Seite 12624-12635
ISSN Quelle:1091-6490
Abstract:In oxygenic photosynthesis, light-driven oxidation of water to molecular oxygen is carried out by the oxygen-evolving complex (OEC) in photosystem II (PS II). Recently, we reported the room-temperature structures of PS II in the four (semi)stable S-states, S1, S2, S3, and S0, showing that a water molecule is inserted during the S2 → S3 transition, as a new bridging O(H)-ligand between Mn1 and Ca. To understand the sequence of events leading to the formation of this last stable intermediate state before O2 formation, we recorded diffraction and Mn X-ray emission spectroscopy (XES) data at several time points during the S2 → S3 transition. At the electron acceptor site, changes due to the two-electron redox chemistry at the quinones, QA and QB, are observed. At the donor site, tyrosine YZ and His190 H-bonded to it move by 50 µs after the second flash, and Glu189 moves away from Ca. This is followed by Mn1 and Mn4 moving apart, and the insertion of OX(H) at the open coordination site of Mn1. This water, possibly a ligand of Ca, could be supplied via a “water wheel”-like arrangement of five waters next to the OEC that is connected by a large channel to the bulk solvent. XES spectra show that Mn oxidation (τ of ∼350 µs) during the S2 → S3 transition mirrors the appearance of OX electron density. This indicates that the oxidation state change and the insertion of water as a bridging atom between Mn1 and Ca are highly correlated.
DOI:doi:10.1073/pnas.2000529117
URL:Bitte beachten Sie: Dies ist ein Bibliographieeintrag. Ein Volltextzugriff für Mitglieder der Universität besteht hier nur, falls für die entsprechende Zeitschrift/den entsprechenden Sammelband ein Abonnement besteht oder es sich um einen OpenAccess-Titel handelt.

Volltext ; Verlag: https://doi.org/10.1073/pnas.2000529117
 Volltext: https://www.pnas.org/content/117/23/12624
 DOI: https://doi.org/10.1073/pnas.2000529117
Datenträger:Online-Ressource
Sprache:eng
Sach-SW:oxygen-evolving complex
 photosynthesis
 photosystem II
 water oxidation
 X-ray free electron laser
K10plus-PPN:1727805062
Verknüpfungen:→ Zeitschrift

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