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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.
非线性光纤方向耦合器孤子动力特性分析 总被引:2,自引:0,他引:2
利用变分方法,导出了双曲正割型光孤子在非线性光纤耦合器中传输时满足的动力学方程组,分析了该方程组的平衡点性态,讨论了光孤子的开关特性.指出参数|β|<2π.是能实现完全的开关操作的必要条件. 相似文献
3.
4.
LI Cun YANG Bai-Feng CAI Hao HUANG Nian-Ning 《理论物理通讯》2006,46(2):244-248
One of the basic problems about the inverse scattering transform for solving a completely integrable nonlinear evolutions equation is to demonstrate that the Jost solutions obtained from the inverse scattering equations of Cauchy integral satisfy the Lax equations. Such a basic problem still exists in the procedure of deriving the dark soliton solutions of the NLS equation in normal dispersion with non-vanishing boundary conditions through the inverse scattering transform. In this paper, a pair of Jost solutions with same analytic properties are composed to be a 2 × 2 matrix and then another pair are introduced to be its right inverse confirmed by the Liouville theorem. As they are both 2 × 2 matrices, the right inverse should be the left inverse too, based upon which it is not difficult to show that these Jost solutions satisfy both the first and second Lax equations. As a result of compatibility condition, the dark soliton solutions definitely satisfy the NLS equation in normal dispersion with non-vanishing boundary conditions. 相似文献
5.
Sean D. Brooks M. F. Mahmood J. A. Donaldson 《Journal of Mathematical Modelling and Algorithms》2004,3(1):19-29
A numerical investigation, based on the split-step Fourier transform algorithm of all optical switching of solitons in a low
birefringent optical fiber is presented. The numerical algorithm is described in detail.
This revised version was published online in August 2006 with corrections to the Cover Date. 相似文献
6.
In the inverse scattering transform (IST), the reflectionless Jost solutions are combined by their analytic properties in the complex spectrum parameter plane, and then can be shown to satisfy the two Lax equations indeed by Liouville theorem. So the corresponding soliton solutions certainly satisfy the nonlinear equation by compatibility condition. Especially the multi-soliton solutions of DNLS equation can be demonstrated in this way.
PACS Numbers: 05.45.Yv, 02.30.-f, 11.10.Ef 相似文献
7.
XIE Bai-Song DU Shu-Cheng 《理论物理通讯》2006,46(10)
Numerical axisymmetric soliton and oscillating wave solutions for the Flierl-Petviashvili equation in plasmas are presented. Solution branch paradigm and examples are given. Some implications of results to ion drift wave as well as force-free field of magnetic equilibrium are briefly discussed. 相似文献
8.
Huai-Dong Cao 《Advances in Mathematics》2007,211(2):794-818
In this paper we prove a compactness result for compact Kähler Ricci gradient shrinking solitons. If (Mi,gi) is a sequence of Kähler Ricci solitons of real dimension n?4, whose curvatures have uniformly bounded Ln/2 norms, whose Ricci curvatures are uniformly bounded from below and μ(gi,1/2)?A (where μ is Perelman's functional), there is a subsequence (Mi,gi) converging to a compact orbifold (M∞,g∞) with finitely many isolated singularities, where g∞ is a Kähler Ricci soliton metric in an orbifold sense (satisfies a soliton equation away from singular points and smoothly extends in some gauge to a metric satisfying Kähler Ricci soliton equation in a lifting around singular points). 相似文献
9.
Christian Erich Zybill Mahmoud Abdel-Hafiez Sami Allam Tharwat El Sherbini 《Progress in Solid State Chemistry》2007,35(2-4):469-480
Ferroelectric thin films form an equilibrium domain structure compatible with their respective crystallographic symmetry. In tetragonal (111) PZT, 90° domains prevail; in (pseudo-tetragonal) (100) SBT both 90° and 180° domains are present. The size of 90° domains has been measured for e.g., PZT as slabs of 15 nm width. Domain size is a result of stress minimization in the film during the paraelectric (PE) → ferroelectric (FE) transition. A precise and regular domain pattern for (111) PZT and (100) SBT films has been investigated in detail by TMSFM. Single domains can be addressed mechanically with the tip of an AFM. Such single domain switching corresponds to a data storage density of 200 Gbit/inch2. Applications of ferroelectric and high- paraelectric materials for e.g., non-volatile data storage replacing DRAM devices or as sensors in infrared cameras are increasingly becoming popular. 相似文献
10.
AO Sheng-Mei YAN Jia-Ren 《理论物理通讯》2007,47(1):15-18
Three types of expression in the dark-soliton perturbation theory based on squared Jost solutions are invesgigaged in ghis paper. It is shown that there are three formally different results about the effects of perturbagion on a dark soliton, and it is proved by means of a transformation between two integral variables that they are essentially equivalent. 相似文献