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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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Stievano I.S. Maio I.A. Canavero F.G. Siviero C. 《Advanced Packaging, IEEE Transactions on》2006,29(1):31-38
This paper addresses the impact of device macromodels on the accuracy of signal integrity and performance predictions for critical digital interconnecting systems. It exploits nonlinear parametric models for both single-ended and differential devices, including the effects of power supply fluctuations and receiver bit detection. The analysis demonstrates that the use of well-designed macromodels dramatically speeds up the simulation as well it preserves timing accuracy even for long bit sequences. 相似文献
5.
K.P. Pipe R.J. Ram 《Photonics Technology Letters, IEEE》2003,15(4):504-506
By measuring the total energy flow from an optical device, we can develop new design strategies for thermal stabilization. Here we present a comprehensive model for heat exchange between a semiconductor laser diode and its environment that includes the mechanisms of conduction, convection, and radiation. We perform quantitative measurements of these processes for several devices, deriving parameters such as a laser's heat transfer coefficient, and then demonstrate the feasibility of thermal probing for the nondestructive wafer-scale characterization of optical devices. 相似文献
6.
Note on B-splines, wavelet scaling functions, and Gabor frames 总被引:3,自引:0,他引:3
Grochenig K. Janssen A.J.E.M. Kaiblinger N. Pfander G.E. 《IEEE transactions on information theory / Professional Technical Group on Information Theory》2003,49(12):3318-3320
Let g be a continuous, compactly supported function on such that the integer translates of g constitute a partition of unity. We show that the Gabor system (g,a,b), with window g and time-shift and frequency-shift parameters a,b>0 has no lower frame bound larger than 0 if b=2,3,... and a>0. In particular, (g,a,b) is not a Gabor frame if g is a continuous, compactly supported wavelet scaling function and if b=2,3,... and a>0. We give an example for our result for the case that g=B/sub 1/, the triangle function supported by [-1,1], by showing pictures of the canonical dual corresponding to (g,a,b) where ab=1/4 and b crosses the lines N=2,3,. 相似文献
7.
de Oliveira J.C. Hosseini M. Shirmohammadi S. Malric F. Nourian S. El Saddik A. Georganas N.D. 《Multimedia, IEEE》2003,10(3):18-29
Using Java-based tools in multimedia collaborative environments accessed over the Internet can increase an application's client base. Most operating systems support Java, and its "compile once-run everywhere" architecture is easy to maintain and update. The Java-based tools presented here let users share Internet resources, including resources originally designed for single use. 相似文献
8.
We propose a standardization procedure that provides a convenient, quantitative and reproducible laboratory-based method for measuring the state of polarization (SOP) fluctuations produced by polarization varying devices. This method is based on the SOP distributions generated by commercial polarization scramblers. We show that these devices generate distributions of the maximum change of the SOP (in a given sample time) that follow Rayleigh statistics, which scale linearly with scrambling frequency and the sample time. We use this procedure to measure the SOP fluctuations in a short length of coiled fiber subject to mechanical perturbations. 相似文献
9.
A common computing-core representation of the discrete cosine transform and discrete sine transform is derived and a reduced-complexity algorithm is developed for computation of the proposed computing-core. A parallel architecture based on the principle of distributed arithmetic is designed further for the computation of these transforms using the common-core algorithm. The proposed scheme not only leads to a systolic-like regular and modular hardware for computing these transforms, but also offers significant improvement in area-time efficiency over the existing structures. The structure proposed here is devoid of complicated input/output mapping and does not involve any complex control. Unlike the convolution-based structures, it does not restrict the transform length to be a prime or multiple of prime and can be utilized as a reusable core for cost-effective, memory-efficient, high-throughput implementation of either of these transforms 相似文献
10.
Piedade M. Sousa L. A. de Almeida T. M. Germano J. da Costa B. A. Lemos J. M. Freitas P. P. Ferreira H. A. Cardoso F. A. 《IEEE transactions on circuits and systems. I, Regular papers》2006,53(11):2384-2395
This paper presents a hand-held microsystem based on new fully integrated magnetoresistive biochips for biomolecular recognition (DNA hybridization, antibody antigen interaction, etc.). Magnetoresistive chip surfaces are chemically treated, enabling the immobilization of probe biomolecules such as DNA or antibodies. Fluid handling is also integrated in the biochip. The proposed microsystem not only integrates the biochip, which is an array of 16times16 magnetoresistive sensors, but it also provides all the electronic circuitry for addressing and reading out each transducer. The proposed architecture and circuits were specifically designed for achieving a compact, programmable and portable microsystem. The microsystem also integrates a hand-held analyzer connected through a wireless channel. A prototype of the system was already developed and detection of magnetic nanoparticles was obtained. This indicates that the system may be used for magnetic label based bioassays 相似文献