Structural evidence for intermediates during O2 formation in photosystem II. Bhowmick, A., Hussein, R., Bogacz, I., Simon, P. S., Ibrahim, M., Chatterjee, R., Doyle, M. D., Cheah, M. H., Fransson, T., Chernev, P., Kim, I., Makita, H., Dasgupta, M., Kaminsky, C. J., Zhang, M., Gätcke, J., Haupt, S., Nangca, I. I., Keable, S. M., Aydin, A. O., Tono, K., Owada, S., Gee, L. B., Fuller, F. D., Batyuk, A., Alonso-Mori, R., Holton, J. M., Paley, D. W., Moriarty, N. W., Mamedov, F., Adams, P. D., Brewster, A. S., Dobbek, H., Sauter, N. K., Bergmann, U., Zouni, A., Messinger, J., Kern, J., Yano, J., & Yachandra, V. K. Nature, 617(7961):629–636, May, 2023. Publisher: Nature Publishing Group
Structural evidence for intermediates during O2 formation in photosystem II [link]Paper  doi  abstract   bibtex   
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 chemistry1–3. 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 transition4–6, 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.
@article{bhowmick_structural_2023,
	title = {Structural evidence for intermediates during {O2} formation in photosystem {II}},
	volume = {617},
	copyright = {2023 The Author(s)},
	issn = {1476-4687},
	url = {https://www.nature.com/articles/s41586-023-06038-z},
	doi = {10.1038/s41586-023-06038-z},
	abstract = {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 chemistry1–3. 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 transition4–6, 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.},
	language = {en},
	number = {7961},
	urldate = {2024-10-16},
	journal = {Nature},
	author = {Bhowmick, Asmit and Hussein, Rana and Bogacz, Isabel and Simon, Philipp S. and Ibrahim, Mohamed and Chatterjee, Ruchira and Doyle, Margaret D. and Cheah, Mun Hon and Fransson, Thomas and Chernev, Petko and Kim, In-Sik and Makita, Hiroki and Dasgupta, Medhanjali and Kaminsky, Corey J. and Zhang, Miao and Gätcke, Julia and Haupt, Stephanie and Nangca, Isabela I. and Keable, Stephen M. and Aydin, A. Orkun and Tono, Kensuke and Owada, Shigeki and Gee, Leland B. and Fuller, Franklin D. and Batyuk, Alexander and Alonso-Mori, Roberto and Holton, James M. and Paley, Daniel W. and Moriarty, Nigel W. and Mamedov, Fikret and Adams, Paul D. and Brewster, Aaron S. and Dobbek, Holger and Sauter, Nicholas K. and Bergmann, Uwe and Zouni, Athina and Messinger, Johannes and Kern, Jan and Yano, Junko and Yachandra, Vittal K.},
	month = may,
	year = {2023},
	note = {Publisher: Nature Publishing Group},
	keywords = {Bioenergetics, Nanocrystallography},
	pages = {629--636},
}
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