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1.
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
2.
对由一类非线性抛物型变分不等方程所描述的无穷维动力系统,给出了存在全局吸引子及弱近似惯性流形的充分条件. 相似文献
3.
4.
The surgery obstruction of a normal map to a simple Poincaré pair (X, Y) lies in the relative surgery obstruction group L *(π 1(Y) → π 1(X)). A well-known result of Wall, the so-called π-π-theorem, states that in higher dimensions a normal map of a manifold with boundary to a simple Poincaré pair with π 1(X) ? π 1(Y) is normally bordant to a simple homotopy equivalence of pairs. In order to study normal maps to a manifold with a submanifold, Wall introduced the surgery obstruction groups LP * for manifold pairs and splitting obstruction groups LS *. In the present paper, we formulate and prove for manifold pairs with boundary results similar to the π-π-theorem. We give direct geometric proofs, which are based on the original statements of Wall’s results and apply obtained results to investigate surgery on filtered manifolds. 相似文献
5.
A functional equation of nonlinear iterates is discussed on the circle S1 for its continuous solutions and differentiable solutions. By lifting to R, the existence, uniqueness and stability of those solutions are obtained. Techniques of continuation are used to guarantee the preservation of continuity and differentiability in lifting. 相似文献
6.
7.
Alfonso Carriazo Luis M. Ferná ndez 《Proceedings of the American Mathematical Society》2004,132(11):3327-3336
In this paper we present an interesting relationship between graph theory and differential geometry by defining submanifolds of almost Hermitian manifolds associated with certain kinds of graphs. We show some results about the possibility of a graph being associated with a submanifold and we use them to characterize CR-submanifolds by means of trees. Finally, we characterize submanifolds associated with graphs in a four-dimensional almost Hermitian manifold.
8.
In this article we use classical formulas involving the K–Bessel function in two variables to express the Poisson kernel on a Riemannian manifold in terms of the heat kernel. We then use the small time asymptotics of the heat kernel on certain Riemannian manifolds to obtain a meromorphic continuation of the associated Poisson kernel to all values of complex time with identifiable singularities. This result reproves in a different setting by different means a well–known theorem due to Duistermaat and Guillemin [DG 75]. Also, we develop analytic expressions for the heat kernel beyond asymptotic expansions. (© 2003 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
9.
S. Azimpour M. Chaichi M. Toomanian 《Journal of Contemporary Mathematical Analysis (Armenian Academy of Sciences)》2007,42(5):270-277
A 4-dimensional Walker metric on a semi Riemanian manifold M, for the canonical metric with c = 0, have been investigated by M. Chaichi, E. García—Río and Y. Matsushita. The paper generalizes these notions to the case of constant c ≠ 0. Specially the form of defining functions of this metric in locally conformally flat 4-dimensional Walker manifolds is found. 相似文献
10.
We prove that a locally compact ANR-space X is a Q-manifold if and only if it has the Disjoint Disk Property (DDP), all points of X are homological Z
∞-points and X has the countable-dimensional approximation property (cd-AP), which means that each map f: K → X of a compact polyhedron can be approximated by a map with the countable-dimensional image. As an application we prove that
a space X with DDP and cd-AP is a Q-manifold if some finite power of X is a Q-manifold. If some finite power of a space X with cd-AP is a Q-manifold, then X
2 and X × [0, 1] are Q-manifolds as well. We construct a countable family χ of spaces with DDP and cd-AP such that no space X ∈ χ is homeomorphic to the Hilbert cube Q whereas the product X × Y of any different spaces X, Y ∈ χ is homeomorphic to Q. We also show that no uncountable family χ with such properties exists.
This work was supported by the Slovenian-Ukrainian (Grant No. SLO-UKR 04-06/07) 相似文献