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1.
2.
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
3.
L. Resse L.G.S. Oliveira C.I.L. de Araujo A.R. Pereira R.L. Silva 《Physics letters. A》2019,383(14):1655-1659
In this work, we have used the MuMax3 software to simulate devices consisting of a ferromagnetic thin film placed over a heavy metal thin film. The devices are two interconnected partial-disks where a Néel domain wall is formed in the disks junction. In our simulations we investigate devices with disk radius nm and different distance d between the disks centers (from nm to nm). By applying strong sinusoidal external magnetic fields, we find a mechanism able to create, annihilate and even manipulate a skyrmion in each side of the device. This mechanism is discussed in terms of interactions between skyrmion and domain wall. The Néel domain wall formed in the center of the device interacts with the Néel skyrmion, leading to a process of transporting a skyrmion from one disk to the other periodically. Our results have relevance for potential applications in spintronics such as logical devices. 相似文献
4.
5.
The structure, chemical composition, and magnetic properties of electrochemically deposited nanocrystalline Co-Ni-Fe films
were investigated using a number of techniques. A high saturation magnetic induction up to B
s
= 21 kG was attained. An enhancement of the saturation magnetization compared to the ideal anticipated one was revealed,
which correlated with the nonlinear behavior of the structural phase composition and lattice parameters with the change of
the composition.
The text was submitted by the authors in English. 相似文献
6.
Experimental data on the effect of thallium and sodium impurities on the lattice heat conductivity of PbTe at room temperature
are reported. Because the lattice of lead chalcogenides is strongly polarized near charged impurities, the effect of impurities
on the lattice heat conductivity depends substantially on their charge state. This property of the material has been used
to determine the charge state of the thallium impurity in PbTe. The results obtained argue for a model of quasi-local thallium-impurity
states which assumes low electron-correlation energy at an impurity center.
Fiz. Tverd. Tela (St. Petersburg) 40, 1206–1208 (July 1998) 相似文献
7.
8.
E. Jackiewicz M. Lukasiak M. Kopcewicz K. Szpila N. Bakun-Czubarow 《Hyperfine Interactions》1992,70(1-4):993-996
Terrestrial basalt rocks considered to be a good analogues of the Martian regolith were studied by using the Mössbauer spectroscopy and X-ray diffraction. The weathering of basalts was followed by the changes of the Fe2+/Fe3+ ratio. The basalt rock undergoes alteration from primary mineral composition (olivine+pyroxene+plagioclase) through smectite to kaolinite clay with oxides and hydroxides with the increase of the Fe2+/Fe3+ ratio. 相似文献
9.
We prove a character formula for any finite-dimensional irreducible representationV of the “queer” Lie superalgebra g=q(n). It expresses chV in terms of the multiplicities of the irreducible g-subquotients of the cohomology groups of certain dominant g-bundles on
the Π-symmetric projective spaces (i.e., on the homogeneous superspacesG/P whose reduced space is a projective space, whereG=Q(n)). We also establish recurrent relations for the above multiplicities, and this enables us to compute explicitly chV for any givenV. This provides a complete solution to the Kac character problem for the Lie superalgebraq(n). Finally, we consider the particular cases ofq(2), q(3), andq(4) in which we compare the new character formula with the generic character formula of [12].
Translated from Itogi Nauki i Tekhniki, Seriya Sovremennaya Matematika i Ee Prilozheniya. Tematicheskie Obzory. Vol. 41, Algebraic
Geometry-7, 1997. 相似文献
10.
A. K. Lopatin 《Ukrainian Mathematical Journal》1997,49(1):51-74
We consider the method of normal forms, the Bogolyubov averaging method, and the method of asymptotic decomposition proposed by Yu. A. Mitropol’skii and the author of this paper. Under certain assumptions about group-theoretic properties of a system of zero approximation, the results obtained by the method of asymptotic decomposition coincide with the results obtained by the method of normal forms or the Bogolyubov averaging method. We develop a new algorithm of asymptotic decomposition by a part of the variables and its partial case — the algorithm of averaging on a compact Lie group. For the first time, it became possible to consider asymptotic expansions of solutions of differential equations on noncommutative compact groups. 相似文献