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Going around the Ko...
Going around the Kok cycle of the water oxidation reaction with femtosecond X-ray crystallography
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- Bhowmick, Asmit (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Simon, Philipp S. (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Bogacz, Isabel (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Hussein, Rana (author)
- Department of Biology, Humboldt-Universität zu Berlin, Berlin, Germany
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- Zhang, Miao (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Makita, Hiroki (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Ibrahim, Mohamed (author)
- Department of Biology, Humboldt-Universität zu Berlin, Berlin, Germany
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- Chatterjee, Ruchira (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Doyle, Margaret D. (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Cheah, Mun Hon (author)
- Uppsala universitet,Molekylär biomimetik
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- Chernev, Petko (author)
- Uppsala universitet,Molekylär biomimetik
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- Fuller, Franklin D. (author)
- Linac Coherent Light Source, SLAC National Accelerator Laboratory, CA, Menlo Park, United States
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- Fransson, Thomas (author)
- Stockholms universitet,Fysikum
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- Alonso-Mori, Roberto (author)
- Linac Coherent Light Source, SLAC National Accelerator Laboratory, CA, Menlo Park, United States
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- Brewster, Aaron S. (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Sauter, Nicolas K. (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Bergmann, Uwe (author)
- Department of Physics, University of Wisconsin-Madison, WI, Madison, United States
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- Dobbek, Holger (author)
- Department of Biology, Humboldt-Universität zu Berlin, Berlin, Germany
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- Zouni, Athina (author)
- Department of Biology, Humboldt-Universität zu Berlin, Berlin, Germany
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- Messinger, Johannes, 1963- (author)
- Uppsala universitet,Umeå universitet,Kemiska institutionen,Molecular Biomimetics, Department of Chemistry-Ångström, Uppsala University, Uppsala, Sweden,Molekylär biomimetik,Department of Chemistry, Umeå University, Umeå SE 90187, Sweden
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- Kern, Jan (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Yachandra, Vittal K. (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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- Yano, Junko (author)
- Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, CA, Berkeley, United States
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(creator_code:org_t)
- International Union Of Crystallography, 2023
- 2023
- English.
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In: IUCrJ. - : International Union Of Crystallography. - 2052-2525. ; 10:6, s. 642-655
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Abstract
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- The water oxidation reaction in photosystem II (PS II) produces most of the molecular oxygen in the atmosphere, which sustains life on Earth, and in this process releases four electrons and four protons that drive the downstream process of CO2 fixation in the photosynthetic apparatus. The catalytic center of PS II is an oxygen-bridged Mn4Ca complex (Mn4CaO5) which is progressively oxidized upon the absorption of light by the chlorophyll of the PS II reaction center, and the accumulation of four oxidative equivalents in the catalytic center results in the oxidation of two waters to dioxygen in the last step. The recent emergence of X-ray free-electron lasers (XFELs) with intense femtosecond X-ray pulses has opened up opportunities to visualize this reaction in PS II as it proceeds through the catalytic cycle. In this review, we summarize our recent studies of the catalytic reaction in PS II by following the structural changes along the reaction pathway via room-temperature X-ray crystallography using XFELs. The evolution of the electron density changes at the Mn complex reveals notable structural changes, including the insertion of OX from a new water molecule, which disappears on completion of the reaction, implicating it in the O-O bond formation reaction. We were also able to follow the structural dynamics of the protein coordinating with the catalytic complex and of channels within the protein that are important for substrate and product transport, revealing well orchestrated conformational changes in response to the electronic changes at the Mn4Ca cluster.
Subject headings
- NATURVETENSKAP -- Biologi -- Strukturbiologi (hsv//swe)
- NATURAL SCIENCES -- Biological Sciences -- Structural Biology (hsv//eng)
- NATURVETENSKAP -- Kemi -- Organisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Organic Chemistry (hsv//eng)
- NATURVETENSKAP -- Biologi -- Biokemi och molekylärbiologi (hsv//swe)
- NATURAL SCIENCES -- Biological Sciences -- Biochemistry and Molecular Biology (hsv//eng)
- NATURVETENSKAP -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)
Keyword
- manganese metalloenzymes
- oxygen evolving complex
- photosystem II
- water-splitting
- wateroxidation
- X-ray free-electron lasers
- X-ray spectroscopy
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Bhowmick, Asmit
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Simon, Philipp S ...
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Bogacz, Isabel
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Hussein, Rana
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Zhang, Miao
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Makita, Hiroki
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Ibrahim, Mohamed
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Chatterjee, Ruch ...
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Doyle, Margaret ...
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Cheah, Mun Hon
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Chernev, Petko
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Fuller, Franklin ...
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Fransson, Thomas
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Alonso-Mori, Rob ...
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Brewster, Aaron ...
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Sauter, Nicolas ...
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Bergmann, Uwe
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Dobbek, Holger
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Zouni, Athina
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Messinger, Johan ...
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Kern, Jan
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Yachandra, Vitta ...
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Yano, Junko
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IUCrJ
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Umeå University
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Stockholm University
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Uppsala University