Untangling the sequence of events during the S2 → S3 transition in photosystem II and implications for the water oxidation mechanism. Ibrahim, M., Fransson, T., Chatterjee, R., Cheah, M. H., Hussein, R., Lassalle, L., Sutherlin, K. D., Young, I. D., Fuller, F. D., Gul, S., Kim, I., Simon, P. S., de Lichtenberg, C., Chernev, P., Bogacz, I., Pham, C. C., Orville, A. M., Saichek, N., Northen, T., Batyuk, A., Carbajo, S., Alonso-Mori, R., Tono, K., Owada, S., Bhowmick, A., Bolotovsky, R., Mendez, D., Moriarty, N. W., Holton, J. M., Dobbek, H., Brewster, A. S., Adams, P. D., Sauter, N. K., Bergmann, U., Zouni, A., Messinger, J., Kern, J., Yachandra, V. K., & Yano, J. Proceedings of the National Academy of Sciences, 117(23):12624–12635, June, 2020. Publisher: Proceedings of the National Academy of Sciences
Untangling the sequence of events during the S2 → S3 transition in photosystem II and implications for the water oxidation mechanism [link]Paper  doi  abstract   bibtex   
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.
@article{ibrahim_untangling_2020,
	title = {Untangling the sequence of events during the {S2} → {S3} transition in photosystem {II} and implications for the water oxidation mechanism},
	volume = {117},
	url = {https://www.pnas.org/doi/10.1073/pnas.2000529117},
	doi = {10.1073/pnas.2000529117},
	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.},
	number = {23},
	urldate = {2024-10-16},
	journal = {Proceedings of the National Academy of Sciences},
	author = {Ibrahim, Mohamed and Fransson, Thomas and Chatterjee, Ruchira and Cheah, Mun Hon and Hussein, Rana and Lassalle, Louise and Sutherlin, Kyle D. and Young, Iris D. and Fuller, Franklin D. and Gul, Sheraz and Kim, In-Sik and Simon, Philipp S. and de Lichtenberg, Casper and Chernev, Petko and Bogacz, Isabel and Pham, Cindy C. and Orville, Allen M. and Saichek, Nicholas and Northen, Trent and Batyuk, Alexander and Carbajo, Sergio and Alonso-Mori, Roberto and Tono, Kensuke and Owada, Shigeki and Bhowmick, Asmit and Bolotovsky, Robert and Mendez, Derek and Moriarty, Nigel W. and Holton, James M. and Dobbek, Holger and Brewster, Aaron S. and Adams, Paul D. and Sauter, Nicholas K. and Bergmann, Uwe and Zouni, Athina and Messinger, Johannes and Kern, Jan and Yachandra, Vittal K. and Yano, Junko},
	month = jun,
	year = {2020},
	note = {Publisher: Proceedings of the National Academy of Sciences},
	pages = {12624--12635},
}
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