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Askerka, Mikhail,Wang, Jimin,Brudvig, Gary W.,Batista, Victor S. American Chemical Society 2014 Biochemistry Vol.53 No.44
<P/><P>The S<SUB>1</SUB> → S<SUB>2</SUB> transition of the oxygen-evolving complex (OEC) of photosystem II does not involve the transfer of a proton to the lumen and occurs at cryogenic temperatures. Therefore, it is commonly thought to involve only Mn oxidation without any significant change in the structure of the OEC. Here, we analyze structural changes upon the S<SUB>1</SUB> → S<SUB>2</SUB> transition, as revealed by quantum mechanics/molecular mechanics methods and the isomorphous difference Fourier method applied to serial femtosecond X-ray diffraction data. We find that the main structural change in the OEC is in the position of the dangling Mn and its coordination environment.</P>
Askerka, Mikhail,Vinyard, David J.,Wang, Jimin,Brudvig, Gary W.,Batista, Victor S. American Chemical Society 2015 Biochemistry Vol.54 No.9
<P>A recent femtosecond X-ray diffraction study produced the first high-resolution structural model of the oxygen-evolving complex of photosystem II that is free of radiation-induced manganese reduction (Protein Data Bank entries <ext-link ext-link-type='pdb' xlink:href='4UB6' xlink:type='simple'>4UB6</ext-link> and <ext-link ext-link-type='pdb' xlink:href='4UB8' xlink:type='simple'>4UB8</ext-link>). We find, however, that the model does not match extended X-ray absorption fine structure and QM/MM data for the S<SUB>1</SUB> state. This is attributed to uncertainty about the positions of oxygen atoms that remain partially unresolved, even at 1.95 Å resolution, next to the heavy manganese centers. In addition, the photosystem II crystals may contain significant amounts of the S<SUB>0</SUB> state, because of extensive dark adaptation prior to data collection.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/bichaw/2015/bichaw.2015.54.issue-9/acs.biochem.5b00089/production/images/medium/bi-2015-00089d_0004.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/bi5b00089'>ACS Electronic Supporting Info</A></P>