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Modeling near-edge ...
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Brena, BarbaraUppsala universitet,Materialteori
(författare)
Modeling near-edge fine structure x-ray spectra of the manganese catalytic site for water oxidation in photosystem II
- Artikel/kapitelEngelska2012
Förlag, utgivningsår, omfång ...
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2012-10-03
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American Chemical Society (ACS),2012
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electronicrdacarrier
Nummerbeteckningar
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LIBRIS-ID:oai:DiVA.org:uu-186074
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https://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-186074URI
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https://doi.org/10.1021/ja306794pDOI
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https://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-106135URI
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https://urn.kb.se/resolve?urn=urn:nbn:se:su:diva-83007URI
Kompletterande språkuppgifter
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Språk:engelska
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Sammanfattning på:engelska
Ingår i deldatabas
Klassifikation
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Ämneskategori:ref swepub-contenttype
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Ämneskategori:art swepub-publicationtype
Anmärkningar
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QC 20121203
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AuthorCount:3;
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The Mn 1s near-edge absorption fine structure (NEXAFS) has been computed by means of transition-state gradient-corrected density functional theory (DFT) on four Mn 4Ca clusters modeling the successive S 0 to S 3 steps of the oxygen-evolving complex (OEC) in photosystem II (PSII). The model clusters were obtained from a previous theoretical study where they were determined by energy minimization. They are composed of Mn(III) and Mn(IV) atoms, progressing from Mn(III) 3Mn(IV) for S 0 to Mn(III) 2Mn(IV) 2 for S 1 to Mn(III)Mn(IV) 3 for S 2 to Mn(IV) 4 for S 3, implying an Mn-centered oxidation during each step of the photosynthetic oxygen evolution. The DFT simulations of the Mn 1s absorption edge reproduce the experimentally measured curves quite well. By the half-height method, the theoretical IPEs are shifted by 0.93 eV for the S 0 → S 1 transition, by 1.43 eV for the S 1 → S 2 transition, and by 0.63 eV for the S 2 → S 3 transition. The inflection point energy (IPE) shifts depend strongly on the method used to determine them, and the most interesting result is that the present clusters reproduce the shift in the S 2 → S 3 transition obtained by both the half-height and second-derivative methods, thus giving strong support to the previously suggested structures and assignments.
Ämnesord och genrebeteckningar
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NATURVETENSKAP Kemi hsv//swe
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NATURAL SCIENCES Chemical Sciences hsv//eng
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Absorption edges
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Absorption fine structure
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Catalytic sites
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Clusters modeling
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Energy minimization
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Fine structures
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Gradient-corrected density functional theory
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Inflection points
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Oxygen evolution
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Oxygen-evolving complexes
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Photosystem II
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Theoretical study
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Transition-state
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Water oxidation
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X-ray spectra
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Catalytic oxidation
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Density functional theory
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Manganese
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oxygen
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water
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article
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catalysis
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chemical structure
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energy
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molecular model
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oxidation
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photosynthesis
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roentgen spectroscopy
Biuppslag (personer, institutioner, konferenser, titlar ...)
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Siegbahn, Per E. M.Stockholms universitet,Fysikum(Swepub:su)ps
(författare)
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Ågren, HansKTH,Teoretisk kemi och biologi(Swepub:kth)u1l2s96v
(författare)
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Uppsala universitetMaterialteori
(creator_code:org_t)
Sammanhörande titlar
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Ingår i:Journal of the American Chemical Society: American Chemical Society (ACS)134:41, s. 17157-171670002-78631520-5126
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