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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.
Paul Bankston 《Archive for Mathematical Logic》2006,45(1):97-112
The Chang-Łoś-Suszko theorem of first-order model theory characterizes universal-existential classes of models as just those
elementary classes that are closed under unions of chains. This theorem can then be used to equate two model-theoretic closure
conditions for elementary classes; namely unions of chains and existential substructures. In the present paper we prove a
topological analogue and indicate some applications. 相似文献
3.
4.
Dan Voiculescu 《Reports on Mathematical Physics》2005,55(1):127-133
This short note summarizes the circumstances of the birth of free probability theory andsome of the recent achievements. 相似文献
5.
本文考察了包括平面上的各种广义 Cantor集 ,Sierpinski集和包括某些连续不可微曲线在内的广义 Sierpinski集 .由相似变换 ,导出了它们的级数表达式 ,并利用它和字符串空间的对应关系 ,计算出它们的Hausdorff维数 相似文献
6.
令H是有限维Hopf代数,A是左H-模代数。本文证明了A是Gorenstein代数的充分必要条件。A^H也是Gorenstein代数的条件。它是Enochs EE,GarciaJJ和del RioA关于群作用相应的理论的推广,同时给出A/A^H是Frobenius扩张的条件。 相似文献
7.
In mononuclear HgI2[(C5H4N)3N], mercury is tetrahedrally coordinated by two nitrogen atoms of a tris(2‐pyridyl)amine ligand and two iodides. The coordination moieties are connected by weak intermolecular Hg(II)···I interactions to give a one‐dimensional structure. Copyright © 2003 John Wiley & Sons, Ltd. 相似文献
8.
We construct a universal space for the class of proper metric spaces of bounded geometry and of given asymptotic dimension. As a consequence of this result, we establish coincidence of asymptotic dimension with asymptotic inductive dimension. 相似文献
9.
O. Yu. Dashkova 《Algebra and Logic》2007,46(5):297-302
We are concerned with infinite-dimensional locally soluble linear groups of infinite central dimension that are not soluble
A3-groups and all of whose proper subgroups, which are not soluble A3-groups, have finite central dimension. The structure of groups in this class is described. The case of infinite-dimensional
locally nilpotent linear groups satisfying the specified conditions is treated separately. A similar problem is solved for
infinite-dimensional locally soluble linear groups of infinite fundamental dimension that are not soluble A3-groups and all of whose proper subgroups, which are not soluble A3-groups, have finite fundamental dimension.
__________
Translated from Algebra i Logika, Vol. 46, No. 5, pp. 548–559, September–October, 2007. 相似文献
10.
D. V. Artamonov 《Mathematical Notes》2007,81(5-6):573-589
A natural criterion for dimensional full-valuedness of locally compact spaces with finitely generated local homology is given. 相似文献