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ABSTRACTQM(UB3LYP)/MM(AMBER) calculations were performed for the locations of the transition structure (TS) of the oxygen–oxygen (O–O) bond formation in the S4 state of the oxygen-evolving complex (OEC) of photosystem II (PSII). The natural orbital (NO) analysis of the broken-symmetry (BS) solutions was also performed to elucidate the nature of the chemical bonds at TS on the basis of several chemical indices defined by the occupation numbers of NO. The computational results revealed a concerted bond switching (CBS) mechanism for the oxygen–oxygen bond formation coupled with the one-electron transfer (OET) for water oxidation in OEC of PSII. The orbital interaction between the σ-HOMO of the Mn(IV)4–O(5) bond and the π*-LUMO of the Mn(V)1=O(6) bond plays an important role for the concerted O–O bond formation for water oxidation in the CaMn4O6 cluster of OEC of PSII. One electron transfer (OET) from the π-HOMO of the Mn(V)1=O(6) bond to the σ*-LUMO of the Mn(IV)4–O(5) bond occurs for the formation of electron transfer diradical, where the generated anion radical [Mn(IV)4–O(5)]-? part is relaxed to the ?Mn(III)4?…?O(5)- structure and the cation radical [O(6)=Mn(V)1]+ ? part is relaxed to the +O(6)–Mn(IV)1? structure because of the charge-spin separation for the electron-and hole-doped Mn–oxo bonds. Therefore, the local spins are responsible for the one-electron reductions of Mn(IV)4->Mn(III)4 and Mn(V)1->Mn(IV)1. On the other hand, the O(5)- and O(6)+ sites generated undergo the O–O bond formation in the CaMn4O6 cluster. The Ca(II) ion in the cubane- skeleton of the CaMn4O6 cluster assists the above orbital interactions by the lowering of the orbital energy levels of π*-LUMO of Mn(V)1=O(6) and σ*-LUMO of Mn(IV)4–O(5), indicating an important role of its Lewis acidity. Present CBS mechanism for the O–O bond formation coupled with one electron reductions of the high-valent Mn ions is different from the conventional radical coupling (RC) and acid-base (AB) mechanisms for water oxidation in artificial and native photosynthesis systems. The proton-coupled electron transfer (PC-OET) mechanism for the O–O bond formation is also touched in relation to the CBS-OET mechanism. 相似文献
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Francis Jordan 《Topology and its Applications》2006,153(14):2386-2412
An abstract scheme using particular types of relations on filters leads to general unifying results on stability under supremum and product of local topological properties. We present applications for Fréchetness, strong Fréchetness, countable tightness and countable fan-tightness, some of which recover or refine classical results, some of which are new. The reader may find other applications as well. 相似文献
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A construction for Segal operations for K-theory of categories with cofibrations, weak equivalences and a biexact pairing is given and coherence properties of the operations are studied. The model for K-theory, which is used, allows coherence to be studied by means of (symmetric) monoidal functors. In the case of Waldhausen A-theory it is shown how to recover the operations used in Waldhausen (Lecture Notes in Mathematics, Vol. 967, Springer, Berlin, 1982, pp. 390-409) for the A-theory Kahn-Priddy theorem. The total Segal operation for A-theory, which assembles exterior power operations, is shown to carry a natural infinite loop map structure. The basic input is the un-delooped model for K-theory, which has been developed from a construction by Grayson and Gillet for exact categories in Gunnarsson et al. (J. Pure Appl. Algebra 79 (1992) 255), and Grayson's setup for operations in Grayson (K-theory (1989) 247). The relevant material from these sources is recollected followed by observations on equivariant objects and pairings. Grayson's conditions are then translated to the context of categories with cofibrations and weak equivalences. The power operations are shown to be well behaved w.r.t. suspension and are extended to algebraic K-theory of spaces. Staying close with the philosophy of Waldhausen (1982) Waldhausen's maps are found. The Kahn-Priddy theorem follows from splitting the “free part” off the equivariant theory. The treatment of coherence of the total operation in A-theory involves results from Laplaza (Lecture Notes in Mathematics, Vol. 281, Springer, Berlin, 1972, pp. 29-65) and restriction to spherical objects in the source of the operation. 相似文献
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A FUNDAMENTAL SOLUTION FOR THE LAPLACE OPERATOR ON THE QUATERNIONIC HEISENBERG GROUP 总被引:2,自引:0,他引:2
朱理 《数学物理学报(B辑英文版)》2002,22(3)
In this paper, the author studies the Laplace operator on the quaternionic Heisenberg group, construct a fundamental solution for it and use this solution to prove the Lp-boundedness and the weak (1-1) boundedness of certain singular convolution operators on the quaternionic Heisenberg group. 相似文献
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The paper provides significant simplifications and extensions of results obtained by Gorsich, Genton, and Strang (J. Multivariate Anal. 80 (2002) 138) on the structure of spatial design matrices. These are the matrices implicitly defined by quadratic forms that arise naturally in modelling intrinsically stationary and isotropic spatial processes. We give concise structural formulae for these matrices, and simple generating functions for them. The generating functions provide formulae for the cumulants of the quadratic forms of interest when the process is Gaussian, second-order stationary and isotropic. We use these to study the statistical properties of the associated quadratic forms, in particular those of the classical variogram estimator, under several assumptions about the actual variogram. 相似文献