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Structural evidence for intermediates during O2 formation in photosystem II

Bhowmick, Asmit (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Hussein, Rana (författare)
Department of Biology, Humboldt Universität zu Berlin, Berlin, Germany
Bogacz, Isabel (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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Simon, Philipp S. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Ibrahim, Mohamed (författare)
Department of Biology, Humboldt Universität zu Berlin, Berlin, Germany; Institute of Molecular Medicine, University of Lübeck, Lübeck, Germany
Chatterjee, Ruchira (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Doyle, Margaret D. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Cheah, Mun Hon (författare)
Uppsala universitet,Molekylär biomimetik
Fransson, Thomas (författare)
KTH,Teoretisk kemi och biologi
Chernev, Petko (författare)
Uppsala universitet,Molekylär biomimetik
Kim, In-Sik (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Makita, Hiroki (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Dasgupta, Medhanjali (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Kaminsky, Corey J. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Zhang, Miao (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Gätcke, Julia (författare)
Department of Biology, Humboldt Universität zu Berlin, Berlin, Germany
Haupt, Stephanie (författare)
Department of Biology, Humboldt Universität zu Berlin, Berlin, Germany
Nangca, Isabela I. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Keable, Stephen M. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Aydin, A. Orkun (författare)
Uppsala universitet,Molekylär biomimetik
Tono, Kensuke (författare)
Japan Synchrotron Radiation Research Institute, Hyogo, Japan; RIKEN SPring-8 Center, Hyogo, Japan
Owada, Shigeki (författare)
Japan Synchrotron Radiation Research Institute, Hyogo, Japan; RIKEN SPring-8 Center, Hyogo, Japan
Gee, Leland B. (författare)
Linac Coherent Light Source, SLAC National Accelerator Laboratory, CA, Menlo Park, United States
Fuller, Franklin D. (författare)
Linac Coherent Light Source, SLAC National Accelerator Laboratory, CA, Menlo Park, United States
Batyuk, Alexander (författare)
Linac Coherent Light Source, SLAC National Accelerator Laboratory, CA, Menlo Park, United States
Alonso-Mori, Roberto (författare)
Linac Coherent Light Source, SLAC National Accelerator Laboratory, CA, Menlo Park, United States
Holton, James M. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States; Department of Biochemistry and Biophysics, University of California, CA, San Francisco, United States; SSRL, SLAC National Accelerator Laboratory, CA, Menlo Park, United States
Paley, Daniel W. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Moriarty, Nigel W. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Mamedov, Fikret, Ph.D., Dr.Sci. (författare)
Uppsala universitet,Molekylär biomimetik
Adams, Paul D. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States; Department of Bioengineering, University of California, CA, Berkeley, United States
Brewster, Aaron S. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Dobbek, Holger (författare)
Department of Biology, Humboldt Universität zu Berlin, Berlin, Germany
Sauter, Nicholas K. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Bergmann, Uwe (författare)
Department of Physics, University of Wisconsin–Madison, WI, Madison, United States,Department of Physics, University of Wisconsin–Madison, Madison, WI, USA
Zouni, Athina (författare)
Department of Biology, Humboldt Universität zu Berlin, Berlin, Germany
Messinger, Johannes, 1963- (författare)
Uppsala universitet,Umeå universitet,Kemiska institutionen,Molecular Biomimetics, Department of Chemistry — Ångström, Uppsala University, Uppsala, Sweden; Department of Chemistry, Umeå University, Umeå, Sweden,Molekylär biomimetik
Kern, Jan (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Yano, Junko (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
Yachandra, Vittal K. (författare)
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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 (creator_code:org_t)
Springer Nature, 2023
2023
Engelska.
Ingår i: Nature. - : Springer Nature. - 0028-0836 .- 1476-4687. ; 617:7961, s. 629-636
Relaterad länk:
https://doi.org/10.1...
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https://umu.diva-por... (primary) (Raw object)
https://uu.diva-port... (primary) (Raw object)
https://urn.kb.se/re...
https://doi.org/10.1...
https://urn.kb.se/re...
https://urn.kb.se/re...
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  • Tidskriftsartikel (refereegranskat)
Abstract Ämnesord
Stäng  
  • In natural photosynthesis, the light-driven splitting of water into electrons, protons and molecular oxygen forms the first step of the solar-to-chemical energy conversion process. The reaction takes place in photosystem II, where the Mn4CaO5 cluster first stores four oxidizing equivalents, the S0 to S4 intermediate states in the Kok cycle, sequentially generated by photochemical charge separations in the reaction center and then catalyzes the O–O bond formation chemistry. Here, we report room temperature snapshots by serial femtosecond X-ray crystallography to provide structural insights into the final reaction step of Kok’s photosynthetic water oxidation cycle, the S3→[S4]→S0 transition where O2 is formed and Kok’s water oxidation clock is reset. Our data reveal a complex sequence of events, which occur over micro- to milliseconds, comprising changes at the Mn4CaO5 cluster, its ligands and water pathways as well as controlled proton release through the hydrogen-bonding network of the Cl1 channel. Importantly, the extra O atom Ox, which was introduced as a bridging ligand between Ca and Mn1 during the S2→S3 transition, disappears or relocates in parallel with Yz reduction starting at approximately 700 μs after the third flash. The onset of O2 evolution, as indicated by the shortening of the Mn1–Mn4 distance, occurs at around 1,200 μs, signifying the presence of a reduced intermediate, possibly a bound peroxide.

Ämnesord

NATURVETENSKAP  -- Biologi -- Biokemi och molekylärbiologi (hsv//swe)
NATURAL SCIENCES  -- Biological Sciences -- Biochemistry and Molecular Biology (hsv//eng)
NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)

Nyckelord

Biology with specialization in Structural Biology

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