Journal
BIOCHEMISTRY
Volume 50, Issue 29, Pages 6308-6311Publisher
AMER CHEMICAL SOC
DOI: 10.1021/bi200681q
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Funding
- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy [DE-SC 000-1423]
- National Institutes of Health (NIH) [GM84267, GM043278, GM32715]
- Grants-in-Aid for Scientific Research [10J02491] Funding Source: KAKEN
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We introduce a quantum mechanics/molecular mechanics model of the oxygen-evolving complex of photosystem II in the S-1 Mn-4(IV,III,IV,III) state, where Ca2+ is bridged to manganese centers by the carboxylate moieties of D170 and A344 on the basis of the new X-ray diffraction (XRD) model recently reported at 1.9 angstrom resolution. The model is also consistent with high-resolution spectroscopic data, including polarized extended X-ray absorption fine structure data of oriented single crystals. Our results provide refined intermetallic distances within the Mn cluster and suggest that the XRD model most likely corresponds to a mixture of oxidation states, including species more reduced than those observed in the catalytic cycle of water splitting.
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