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61.
We present an extension of some popular hindered rotor (HR) models, namely, the one-dimensional HR (1DHR) and the degenerated two-dimensional HR (d2DHR) models, allowing for a simple and accurate treatment of internal rotations. This extension, based on the use of a variable kinetic function in the Hamiltonian instead of a constant reduced moment of inertia, is extremely suitable in the case of rocking/wagging motions involved in dissociation or atom transfer reactions. The variable kinetic function is first introduced in the framework of a classical 1DHR model. Then, an effective temperature and potential dependent constant is proposed in the cases of quantum 1DHR and classical d2DHR models. These methods are finally applied to the atom transfer reaction SiCl(3)+BCl(3)→SiCl(4)+BCl(2). We show, for this particular case, that a proper accounting of internal rotations greatly improves the accuracy of thermodynamic and kinetic predictions. Moreover, our results confirm (i) that using a suitably defined kinetic function appears to be very adapted to such problems; (ii) that the separability assumption of independent rotations seems justified; and (iii) that a quantum mechanical treatment is not a substantial improvement with respect to a classical one. 相似文献
62.
Gomila A Le Poul N Cosquer N Kerbaol JM Noël JM Reddy MT Jabin I Reinaud O Conan F Le Mest Y 《Dalton transactions (Cambridge, England : 2003)》2010,39(48):11516-11518
We report the self-induced "electroclick" immobilization of the [Cu(II)(6-ethynyl-TMPA)(H(2)O)](2+) complex, by its simple electro-reduction, onto a mixed azidoundodecane-/decane-thiol modified gold electrode. The redox response of the grafted [Cu(II/I)(TMPA)] at the modified electrode is fully reversible indicating no Cu coordination change and a fast electron transfer. 相似文献
63.
Lameiras P Boudesocque L Mouloungui Z Renault JH Wieruszeski JM Lippens G Nuzillard JM 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2011,212(1):161-168
NMR of weakly polar analytes in an apolar ultraviscous solvent has recently been proposed for mixture analysis as a pertinent alternative to the DOSY experiment. The present article reports the first use of glycerol and glycerol carbonate as polar solvents for the NMR analysis of a model mixture of dipeptides. This work demonstrates the high potentiality of these solvents for the analysis of mixtures made of polar and potentially bioactive compounds. Medium-sized molecules slowly reorient in glycerol and glycerol carbonate under particular temperature conditions, so that solute resonances may show spin diffusion in NOESY spectra, thus opening the way to mixture analysis. Glycerol and glycerol carbonate have turned out to be ultraviscous solvents of choice for the individualization of four structurally close mixed dipeptides: Leu-Val, Leu-Tyr, Gly-Tyr and Ala-Tyr by means of 1D and 2D NOESY experiments. Selective sample excitation and signal detection were implemented to eliminate the intense proton signals of the non-deuterated solvents. Moreover, the recording of a multiplet selective 2D NOESY-TOCSY has shown that the analytical power of NMR in highly viscous solvents is not limited to the extraction of mixture component 1D subspectra but may also yield some supplementary information about atom connectivity within components. 相似文献
64.
Kumar R Spuesens T Mechet P Kumar P Raz O Olivier N Fedeli JM Roelkens G Baets R Van Thourhout D Morthier G 《Optics letters》2011,36(13):2450-2452
Using a 7.5 μm diameter disk fabricated with III-V-on-silicon fabrication technology, we demonstrate bias-free all-optical wavelength conversion for non-return-to-zero on-off keyed pseudorandom bit sequence (PRBS) data at the speed of 10 Gbits/s with an extinction ratio of more than 12 dB. The working principle of such a wavelength converter is based on free-carrier-induced refractive index modulation in a pump-probe configuration. We believe it to be the first bias-free on-chip demonstration of all-optical wavelength conversion using PRBS data. All-optical gating measurements in the pump-probe configuration with the same device have revealed that it is possible to achieve wavelength conversion beyond 20 Gbits/s. 相似文献
65.
José Aliste-Prieto Daniel Coronel Jean-Marc Gambaudo 《Communications in Mathematical Physics》2011,306(2):365-380
This paper concerns self-similar tilings of the Euclidean plane. We consider the number of occurrences of a given tile in
any domain bounded by a Jordan curve. For a large class of self-similar tilings, including many well-known examples, we give
estimates of the oscillation of this number of occurrences around its average frequency times the total number of tiles in
the domain, which depend only on the Jordan curve. 相似文献
66.
The goal programming (GP) model is probably the best known in mathematical programming with multiple objectives. Available in various versions, GP is one of the most powerful multiple objective methods which has been applied in much varied fields. It has also been the target of many criticisms among which are those related to the difficulty of determining precisely the goal values as well as those concerning the decision-maker's near absence in this modelling process. In this paper, we will use the concept of indifference thresholds for modelling the imprecision related to the goal values. Many classical imprecise and fuzzy GP model formulations can be considered as a particular case of the proposed formulation. 相似文献
67.
We present low complexity models for the transport of passive scalars for environmental applications. The model uses partial observations assimilation. Similitude solutions are proposed in a non symmetric metric based on travel times. The approach does not require the solution of any PDE and is mesh free. Also, the solution can be computed in one point only without computing the whole solution. To cite this article: B. Mohammadi, J.-M. Brun, C. R. Mecanique 334 (2006). 相似文献
68.
Akio Maeda Jun Sasaki Jean-Marc Pfefferl Yoshinori Shichida Tru Yoshizawa 《Photochemistry and photobiology》1991,54(6):911-921
Abstract– Difference Fourier transform infrared spectra were recorded for bacteriorhodopsin upon irradiation at 230, 170 or 77 K, which gave, respectively, the spectrum of the M, L or K intermediate minus unphotolyzed all-trans bacteriorhodopsin (denoted as BR). By replacement of the Schiff base nitrogen with 15N, or of either its hydrogen at N or C15 with deuterium, the vibrational bands related to the Schiff base were identified and the isotope-shifts evaluated for BR, K and L. The 1348 cm?l band of BR and K and the 1400 cm?1 band of L were sensitive to each of these isotope substitutions. The 1254 cm?1 band of BR, the 1245 cm?1 band of K and the 1301 cm?1 band of L were sensitive to either N- or C15-deuteration but not to 15N-substitution. The N—D in-plane bending vibration of K and L appeared at 969 and 997 cm?1, respectively, upon substitution with D2O. All the results show that L is larger in frequencies related to the N—H in-plane bending vibration than K or BR and suggest that L has the strongest interaction with the protein. Among the bands containing an N—H bending vibration, the 1348 cm?1 band of K was more intense than the corresponding band of L at 1400 cm?1. The C15-deuteration-induced upshift of the 1245 cm?1 band of K was unobservable for the 1301 cm?1 band of L. Such differences between L and K might be brought about by a distortion in the retinal moiety close to the protonated Schiff base of the 13-cis chromophore. 相似文献
69.
Yu Shen Jean-Yves Potvin Jean-Marc Rousseau Serge Roy 《Annals of Operations Research》1995,61(1):189-211
In this paper, we describe an expert consulting system for a dispatcher working in a courier service company. The system integrates interactive-graphic features and a learning module to support the dispatcher in his(her) task, and to suggest appropriate decisions when new requests come in. An experiment with a professional dispatcher is also reported. 相似文献