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951.
Lee VY Fukawa T Nakamoto M Sekiguchi A Tumanskii BL Karni M Apeloig Y 《Journal of the American Chemical Society》2006,128(35):11643-11651
((t)Bu(2)MeSi)(2)Sn=Sn(SiMe(t)Bu(2))(2) 1, prepared by the reaction of (t)Bu(2)MeSiNa with SnCl(2)-diox in THF and isolated as dark-green crystals, represents the first example of acyclic distannene with a Sn=Sn double bond that is stable both in the crystalline form and in solution. This was proved by the crystal and NMR spectral data of 1. Distannene 1 has these peculiar structural features: a shortest among all acyclic distannenes Sn=Sn double bond of 2.6683(10) A, a nearly planar geometry around both Sn atoms, and a highly twisted Sn=Sn double bond. The reactions of 1 toward carbon tetrachloride and phenylacetylene also correspond to the reactivity anticipated for the Sn=Sn double bond. The one-electron reduction of 1 with potassium produced the distannene anion radical, the heavy analogue of alkene ion radicals, for which the particular crystal structure and low-temperature EPR behavior are also discussed. 相似文献
952.
We present a simple and efficient method for calculating symmetrized time correlation functions of neat quantum fluids. Using the pair-product approximation to each complex-time quantum mechanical propagator, symmetrized correlation functions are written in terms of a double integral for each degree of freedom with a purely positive integrand. At moderate temperatures and densities, where the pair-product approximation to the Boltzmann operator is sufficiently accurate, the method leads to quantitative results for the early time part of the correlation function. The method is tested extensively on liquid para-hydrogen at 25 K and used to obtain accurate quantum mechanical results for the initial 0.2 ps segment of the symmetrized velocity autocorrelation function of this system, as well as the incoherent dynamic structure factor at certain momentum transfer values. 相似文献
953.
The authors applied the time dependent density functional method (TDDFM) and a linear model to solvation dynamics in simple binary solvents. Changing the solute-solvent interactions at t=0, the authors calculated the time evolution of density fields for solvent particles after the change (t>0) by the TDDFM and linear model. First, the authors changed the interaction of only one component of solvents. In this case, the TDDFM showed that the solvation time decreased monotonically with a mole fraction of the solvent strongly interacting with the solute. The monotonical decreases agreed with experimental results, while the linear model did not reproduce these results. The authors also calculated the solvation time by changing the interaction of both components. The calculation showed that the mole fraction dependence had the peak. The TDDFM presented a much higher peak than the linear model. The difference between the TDDFM and the linear model was caused by a nonlinear effect on an exchange process of solvent particles. 相似文献
954.
[reaction: see text] Herein we describe a novel Co(2)(CO)(8)-catalyzed intramolecular aza-Pauson-Khand-type reaction of alkynecarbodiimide derivatives affords pyrrolo[2,3-b]indol-2-one ring systems in reasonable yields. This is the first reported Co(2)(CO)(8) successfully applied in the hetero-Pauson-Khand reaction. Significantly, the transformation of one of our pyrrolo[2,3-b]indol-2-one derivatives into the indole alkaloid, (+/-)-physostigmine, was completed in a highly stereoselective manner. 相似文献
955.
Yamanaka S Kubo A Inumaru K Komaguchi K Kini NS Inoue T Irifune T 《Physical review letters》2006,96(7):076602
Single crystals of three-dimensional (3D) C60 polymer were prepared by the topotactic conversion of two-dimensional (2D) C60 polymer single crystals at a pressure of 15 GPa at 600 degrees C. The x-ray single crystal study revealed that the 3D C60 polymer crystallized in a body centered orthorhombic space group Immm, and spherical C60 monomer units were substantially deformed to rectangular parallelepiped (cuboidal) shapes, each unit being bonded to eight cuboidal C60 neighbors via [3 + 3] cycloaddition. The 3D C60 polymer was electron conductive, in contrast with the nonconductive behavior of 2D polymers. 相似文献
956.
Yoshida T Kajino T Yokomakura H Kimura K Takamura A Hartmann DH 《Physical review letters》2006,96(9):091101
Light element synthesis in supernovae through neutrino-nucleus interactions, i.e., the v process, is affected by neutrino oscillations in the supernova environment. There is a resonance of 13-mixing in the O/C layer, which increases the rates of charged-current -process reactions in the outer He-rich layer. The yields of 7Li and 11B increase by about a factor of 1.9 and 1.3, respectively, for a normal mass hierarchy and an adiabatic 13-mixing resonance, compared to those without neutrino oscillations. In the case of an inverted mass hierarchy and a nonadiabatic 13-mixing resonance, the increase in the 7Li and 11B yields is much smaller. Observations of the 7Li/11B ratio in stars showing signs of supernova enrichment could thus provide a unique test of neutrino oscillations and constrain their parameters and the mass hierarchy. 相似文献
957.
A natural extension of the cohomology suspension to a free loop space is constructed from the evaluation map and is shown to have good properties in cohomology calculation. This map is generalized to a twisted loop space which is a space of paths twisted by a given self-map of the underlying space. As an application, the cohomology of free and twisted loop spaces of classifying spaces of compact Lie groups, including some finite Chevalley groups, is calculated. 相似文献
958.
A cycle of order is called a -cycle. A non-induced cycle is called a chorded cycle. Let be an integer with . Then a graph of order is chorded pancyclic if contains a chorded -cycle for every integer with . Cream, Gould and Hirohata (Australas. J. Combin. 67 (2017), 463–469) proved that a graph of order satisfying for every pair of nonadjacent vertices , in is chorded pancyclic unless is either or , the Cartesian product of and . They also conjectured that if is Hamiltonian, we can replace the degree sum condition with the weaker density condition
and still guarantee the same conclusion. In this paper, we prove this conjecture by showing that if a graph of order with contains a -cycle, then contains a chorded -cycle, unless and is either or , Then observing that and are exceptions only for , we further relax the density condition for sufficiently large . 相似文献
959.
Haruko Ikeuchi Mitsuhiro Kanakubo Shin Okuno Rika Sato Koichi Fujita Manatsu Hamada Nobuhiro Shoda Kenta Fukui Koji Okada Hikaru Kanazawa Akira Iimori Daisaku Miyake Takeshi Takeda Gen P. Satô 《Journal of solution chemistry》2010,39(10):1428-1453
The densities and the viscosities of tris(acetylacetonato)cobalt(III) solutions in acetonitrile, dichloromethane, chloroform, tetrachloromethane, benzene, toluene, ethylbenzene, and p-xylene were measured in the dilute concentration regions at several temperatures ranging from 278 to 313 K under ambient pressure. The partial molar volumes of the solvents and solute were calculated. They are independent of concentration and increase slightly as the temperature increases. The viscosity A- and B-coefficients of the Jones-Dole equation were obtained. The A-coefficients were found to be zero within experimental error. The B-coefficients are positive and decrease as the temperature increases. Thermodynamic quantities of activation for viscous flow were calculated on the basis of Eyring’s viscosity equation. From the quantities obtained in this study, along with some information from the literature, it is suggested that structure-making interactions occur between the segments of the complex and the solvent molecules. These interactions include electrostatic interactions between the local charge on the complex and the dipole moment of the solvent in solutions of acetonitrile and dichloromethane, interlocking packing interactions along C 3-axis of the complex with solvent in solutions of chloroform and tetrachloromethane, and π-electron interactions between the chelate ring of the complex and the solvent in solutions of benzene, toluene, ethylbenzene, and p-xylene. 相似文献
960.
Two Janus [2]rotaxanes, 5a and 5b , with α‐cyclodextrin (α‐CD) derivatives substituted on the 6‐position with two recognition sites (azobenzene and heptamethylene (C7)) that were linked with linkers of different lengths (oligo(ethylene glycol) with a degree of polymerization equal to 2 or approximately 21) were synthesized and characterized. 2D ROESY NMR spectroscopy and circular dichroism (cd) spectra demonstrated that the recognition site of the α‐CD moiety was switched by photoisomerization of the azobenzene moiety in 5a and 5b . The different size changes of 5a and 5b in hydrodynamic radius (RH) owing to the different length of linker between two recognition sites were observed by pulse‐field‐gradient spin‐echo NMR spectroscopy. The kinetic results indicated that the different length of linker had no or a weak effect for the photoisomerization process of 5a and 5b . 相似文献