2006
DOI: 10.1016/j.jinorgbio.2006.01.017
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Characterization of synthetic oxomanganese complexes and the inorganic core of the O2-evolving complex in photosystem II: Evaluation of the DFT/B3LYP level of theory

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Cited by 103 publications
(108 citation statements)
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References 121 publications
(173 reference statements)
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“…While the S-states are well established, the structure of the catalytic metal cluster along the cycle and its ligation scheme remain poorly understood. Computational modeling studies (Blomberg et al 1997;Lundberg et al 2003;McEvoy & Brudvig 2004;Siegbahn 2002;Siegbahn & Crabtree 1999;Siegbahn & Lundberg 2005;Siegbahn & Lundberg 2006;Sproviero et al 2006a;Sproviero et al 2006b;Sproviero et al 2007c), based on density functional (DFT) theory and quantum mechanics/molecular mechanics (QM/MM) hybrid methods, have recently proposed energetically minimized and chemically satisfactory models of the fully ligated OEC within PSII, maximally consistent with experimental results. The computational models are useful for rationalizing a structure-based mechanism of water splitting in PSII as described by the OEC oxidation intermediate states.…”
Section: Introductionmentioning
confidence: 77%
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“…While the S-states are well established, the structure of the catalytic metal cluster along the cycle and its ligation scheme remain poorly understood. Computational modeling studies (Blomberg et al 1997;Lundberg et al 2003;McEvoy & Brudvig 2004;Siegbahn 2002;Siegbahn & Crabtree 1999;Siegbahn & Lundberg 2005;Siegbahn & Lundberg 2006;Sproviero et al 2006a;Sproviero et al 2006b;Sproviero et al 2007c), based on density functional (DFT) theory and quantum mechanics/molecular mechanics (QM/MM) hybrid methods, have recently proposed energetically minimized and chemically satisfactory models of the fully ligated OEC within PSII, maximally consistent with experimental results. The computational models are useful for rationalizing a structure-based mechanism of water splitting in PSII as described by the OEC oxidation intermediate states.…”
Section: Introductionmentioning
confidence: 77%
“…Therefore, the resulting models circumvent the effect of radiation damage caused by reduction of the Mn centers in the description of the OEC configuration. The implemented computational methodology has been rigorously tested with well-characterized manganese model compounds, verifying its ability to predict highly accurate XRD geometries (Sproviero et al 2006a). Therefore, the resulting DFT-QM/MM structures are expected to benefit the construction of a complete model of the water splitting catalytic cycle in terms of detailed molecular structures of the OEC catalytic intermediates (Sproviero et al 2007e).…”
Section: Structure and Mechanism Of The Oecmentioning
confidence: 99%
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“…These results can be rationalized by noting that charge transfer between manganese ions and ligand/oxo-bridges affects the net ionic charges of metal centres, complicating the correlation with formal oxidation numbers (Sproviero et al 2006a(Sproviero et al ,b, 2007. The underlying charge-transfer delocalization process is common to synthetic oxomanganese complexes (Sproviero et al 2006b) and partially neutralizes the net ionic charges of the metal centres, leaving a smaller positive charge on Mn(4) (qZC1.35) than on Ca 2C (qZC1.77; table 1). Therefore, it is not surprising that W slow is attached to Ca 2C , as indicated by the energetic analysis of figure 3, even when such a metal centre has a smaller oxidation number than Mn(4).…”
Section: Cp43-r357 Membrane Normalmentioning
confidence: 99%