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  • Kern, JanLawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)

Structures of the intermediates of Kok’s photosynthetic water oxidation clock

  • Article/chapterEnglish2018

Publisher, publication year, extent ...

  • 2018-11-07
  • Nature Publishing Group,2018
  • printrdacarrier

Numbers

  • LIBRIS-ID:oai:DiVA.org:umu-153920
  • https://urn.kb.se/resolve?urn=urn:nbn:se:umu:diva-153920URI
  • https://doi.org/10.1038/s41586-018-0681-2DOI
  • https://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-371878URI

Supplementary language notes

  • Language:English
  • Summary in:English

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  • Subject category:ref swepub-contenttype
  • Subject category:art swepub-publicationtype

Notes

  • Inspired by the period-four oscillation in flash-induced oxygen evolution of photosystem II discovered by Joliot in 1969, Kok performed additional experiments and proposed a five-state kinetic model for photosynthetic oxygen evolution, known as Kok’s S-state clock or cycle1,2. The model comprises four (meta)stable intermediates (S0, S1, S2 and S3) and one transient S4 state, which precedes dioxygen formation occurring in a concerted reaction from two water-derived oxygens bound at an oxo-bridged tetra manganese calcium (Mn4CaO5) cluster in the oxygen-evolving complex3–7. This reaction is coupled to the two-step reduction and protonation of the mobile plastoquinone QB at the acceptor side of PSII. Here, using serial femtosecond X-ray crystallography and simultaneous X-ray emission spectroscopy with multi-flash visible laser excitation at room temperature, we visualize all (meta)stable states of Kok’s cycle as high-resolution structures (2.04–2.08 Å). In addition, we report structures of two transient states at 150 and 400 µs, revealing notable structural changes including the binding of one additional ‘water’, Ox, during the S2→S3 state transition. Our results suggest that one water ligand to calcium (W3) is directly involved in substrate delivery. The binding of the additional oxygen Ox in the S3 state between Ca and Mn1 supports O–O bond formation mechanisms involving O5 as one substrate, where Ox is either the other substrate oxygen or is perfectly positioned to refill the O5 position during O2 release. Thus, our results exclude peroxo-bond formation in the S3 state, and the nucleophilic attack of W3 onto W2 is unlikely.

Subject headings and genre

Added entries (persons, corporate bodies, meetings, titles ...)

  • Chatterjee, RuchiraLawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Young, Iris D.Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Fuller, Franklin D.Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Lassalle, LouiseLawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Ibrahim, MohamedHumboldt Univ, Inst Biol, Berlin, Germany (author)
  • Gul, SherazLawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Fransson, ThomasSLAC Natl Accelerator Lab, Stanford PULSE Inst, Menlo Pk, CA USA;Heidelberg Univ, Interdisciplinary Ctr Sci Comp, Heidelberg, Germany (author)
  • Brewster, Aaron S.Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Alonso-Mori, RobertoSLAC Natl Accelerator Lab, LCLS, Menlo Pk, CA USA (author)
  • Hussein, RanaHumboldt Univ, Inst Biol, Berlin, Germany (author)
  • Zhang, MiaoHumboldt Univ, Inst Biol, Berlin, Germany (author)
  • Douthit, LaceyLawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • de Lichtenberg, CasperUppsala universitet,Umeå universitet,Kemiska institutionen,Department of Chemistry—Ångström, Molecular Biomimetics, Uppsala University, Uppsala, Sweden,Molekylär biomimetik,Umeå Univ, Kemiskt Biol Ctr, Inst Kemi, Umeå, Sweden(Swepub:uu)casde246 (author)
  • Cheah, Mun HonUppsala universitet,Molekylär biomimetik(Swepub:uu)munch343 (author)
  • Shevela, DmitriyUmeå universitet,Kemiska institutionen,Umea Univ, Kemiskt Biol Ctr, Inst Kemi, Umea, Sweden(Swepub:umu)dmsh0004 (author)
  • Wersig, JuliaHumboldt Univ, Inst Biol, Berlin, Germany (author)
  • Seuffert, InaHumboldt Univ, Inst Biol, Berlin, Germany (author)
  • Sokaras, DimosthenisSLAC Natl Accelerator Lab, SSRL, Menlo Pk, CA USA (author)
  • Pastor, ErnestLawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Weninger, ClemensSLAC Natl Accelerator Lab, LCLS, Menlo Pk, CA USA (author)
  • Kroll, ThomasSLAC Natl Accelerator Lab, SSRL, Menlo Pk, CA USA (author)
  • Sierra, Raymond G.SLAC Natl Accelerator Lab, LCLS, Menlo Pk, CA USA (author)
  • Aller, PierreDiamond Light Source Ltd, Harwell Sci & Innovat Campus, Didcot, Oxon, England (author)
  • Butryn, AgataDiamond Light Source Ltd, Harwell Sci & Innovat Campus, Didcot, Oxon, England (author)
  • Orville, Allen M.Diamond Light Source Ltd, Harwell Sci & Innovat Campus, Didcot, Oxon, England (author)
  • Liang, MengningSLAC Natl Accelerator Lab, LCLS, Menlo Pk, CA USA (author)
  • Batyuk, AlexanderSLAC Natl Accelerator Lab, LCLS, Menlo Pk, CA USA (author)
  • Koglin, Jason E.SLAC Natl Accelerator Lab, LCLS, Menlo Pk, CA USA (author)
  • Carbajo, SergioSLAC Natl Accelerator Lab, LCLS, Menlo Pk, CA USA (author)
  • Boutet, SébastienSLAC Natl Accelerator Lab, LCLS, Menlo Pk, CA USA (author)
  • Moriarty, Nigel W.Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Holton, James M.Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA;SLAC Natl Accelerator Lab, SSRL, Menlo Pk, CA USA;Univ Calif San Francisco, Dept Biochem & Biophys, San Francisco, CA 94143 USA (author)
  • Dobbek, HolgerHumboldt Univ, Inst Biol, Berlin, Germany (author)
  • Adams, Paul D.Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA;Univ Calif Berkeley, Dept Bioengn, Berkeley, CA 94720 USA (author)
  • Bergmann, UweSLAC Natl Accelerator Lab, Stanford PULSE Inst, Menlo Pk, CA USA (author)
  • Sauter, Nicholas K.Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Zouni, AthinaHumboldt Univ, Inst Biol, Berlin, Germany (author)
  • Messinger, JohannesUppsala universitet,Umeå universitet,Kemiska institutionen,Molekylär biomimetik,Umeå Univ, Kemiskt Biol Ctr, Inst Kemi, Umeå, Sweden(Swepub:uu)johme269 (author)
  • Yano, JunkoLawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Yachandra, Vittal K.Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA (author)
  • Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USAHumboldt Univ, Inst Biol, Berlin, Germany (creator_code:org_t)

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  • In:Nature: Nature Publishing Group563, s. 421-4250028-08361476-4687

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