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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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P. Cofta 《BT Technology Journal》2006,24(2):214-218
Trust is the key element of commerce, both for traditional models and — more recently — for eCommerce. Unlike its traditional
counterpart, eCommerce relies on trust being created and maintained with the help of digital devices and services. Convergence
brings significant changes to the way people interact through digital media by offering ubiquitous and seamless communication.
This has a significant impact on the way trust is established and maintained, with consequent impact upon eCommerce. This
paper identifies a number of the most important challenges to trust in eCommerce as well as trust-related aspects of key enablers
of eCommerce. From this perspective, the paper studies an impact of convergence on trust within eCommerce to identify several
positive relationships. 相似文献
6.
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
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Performance study of iSCSI-based storage subsystems 总被引:9,自引:0,他引:9
iISCSI is emerging as an end-to-end protocol for transporting storage I/O block data over IP networks. By exploiting the ubiquitous Internet infrastructure, iSCSI greatly facilitates remote storage, remote backup, and data mirroring. This article evaluates the performance of two typical iSCSI storage subsystems by measuring and analyzing block-level I/O access performance and file-level access performance. In the file-level performance study, we compare file access performance in an NAS scheme with that in an iSCSI-based SAN scheme. Our test results show that Gigabit Ethernet-based iSCSI can reach very high bandwidth, close to that of a direct FC disk access in block I/O access. However, when the iSCSI traverses through longer distance, throughput relies heavily on the available bandwidth between the initiator and the target. On the other hand, the file-level performance shows that iSCSI-based file access (SAN scheme) provides higher performance than using NFS protocol in Linux and SMB protocol in Windows (NAS scheme). However, the advantage of using iSCSI-based file accesses decreases as the file size increases. The obtained experimental results shed some light on the performance of applications based on iSCSI storage. 相似文献
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L. Gao P. Hrter Ch. Linsmeier J. Gstttner R. Emling D. Schmitt-Landsiedel 《Materials Science in Semiconductor Processing》2004,7(4-6):331
Deposition of Ag films by direct liquid injection-metal organic chemical vapor deposition (DLI-MOCVD) was chosen because this preparation method allows precise control of precursor flow and prevents early decomposition of the precursor as compared to the bubbler-delivery. Silver(I)-2,2-dimethyl-6,6,7,7,8,8,8-heptafluoro-3,5-octanedionato-triethylphosphine [Ag(fod)(PEt3)] as the precursor for Ag CVD was studied, which is liquid at 30 °C. Ag films were grown on different substrates of SiO2/Si and TiN/Si. Argon and nitrogen/hydrogen carrier gas was used in a cold wall reactor at a pressure of 50–500 Pa with deposition temperature ranging between 220 °C and 350 °C. Ag films deposited on a TiN/Si diffusion barrier layer have favorable properties over films deposited on SiO2/Si substrate. At lower temperature (220 °C), film growth is essentially reaction-limited on SiO2 substrate. Significant dependence of the surface morphology on the deposition conditions exists in our experiments. According to XPS analysis pure Ag films are deposited by DLI-MOCVD at 250 °C by using argon as carrier gas. 相似文献
9.
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
10.
Popular biorthogonal wavelet filters via a lifting scheme and its application in image compression 总被引:2,自引:0,他引:2
Cheng L. Liang D.L. Zhang Z.H. 《Vision, Image and Signal Processing, IEE Proceedings -》2003,150(4):227-232
A technique using a lifting scheme is presented for constructing compactly supported wavelets whose coefficients are composed of free variables locating in an interval. An efficient approach-based wavelet for image compression is developed by selecting the coefficients of the 9-7 wavelet filter and associated lifting scheme. Furthermore, the rationalised coefficients wavelet filter that can be implemented with simple integer arithmetic is achieved and its characteristic is close to the well known original irrational coefficients 9-7 wavelet filters developed by A. Cohen et al. (Commun. Pure Appl. Maths., vol.45, no.1, p.485-560, 1992). To reduce the computational cost of image coding applications further, an acceleration technique is proposed for the lifting steps. Software and hardware simulations show that the new method has very low complexity, and simultaneously preserves the high quality of the compressed image. 相似文献