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Y. Pomeau S. Zaleski P. Manneville 《Zeitschrift für Angewandte Mathematik und Physik (ZAMP)》1985,36(3):367-394
For an axisymmetric cellular structure of wavenumberq
0, the amplitude of the first linearly unstable mode is proportional to the Bessel functionJ
0(q
0r). If the radius of the structure is much larger thanq
0
–1
, the first mode has a large relative maximum near the center. The nonlinear saturation of this instability gives an amplitude of order 1/2, being the small growth rate of the linear instability. The saturation amplitude near the center is of order 1/4. This prediction is confirmed by numerical analysis and numbers are given to make possible a comparison with the Rayleigh-Bénard instability.
Resumé Pour une structure cellulaire axisymétrique de nombre d'ondeq 0, l'amplitude du premier mode instable est proportioneile á la fonction de BesselJ 0(q 0r). Si le rayon de la structure est très supérieur àq 0 –1 ce premier mode a un grand maximum relatif au centre. La saturation non linéaire de cette instabilité conduit à une amplitude en 1/2 ( taux de croissance-petit-de l'instabilité linéaire). L'amplitude de saturation au centre est d'ordre 1/4. Cette prédiction est confirmée par l'analyse numérique, et les nombres nécessaires à la comparaison avec l'instabilité de Rayleigh-Bénard sont donnés.相似文献
44.
Cécile Appert John F. Olson Daniel H. Rothman Stéphane Zaleski 《Journal of statistical physics》1995,81(1-2):181-197
The dynamics of phase separation is explored using an immiscible 3D lattice-gas model. Scaling laws for the growth rate and power spectraS(k) of the growth patterns are computed. For small wavenumbersS(k) shows a crossover fromk
2 tok
4 behavior. The theoretical prediction for the asymptotic domain growthRt
2/3 is supported by our results. We discuss the possibility to observe an intermediatet scaling. We show the influence of hydrodynamic forces in symmetric and asymmetric mixtures by comparing simulations with and without momentum conservation. The structure functionS(k) is not significantly modified by hydrodynamics, but the growth rate changes clearly. As a general result, it is shown that, in spite of the unusual thermodynamics of this model, many characteristics of the growth dynamics are surprisingly in agreement with the classical theoretical and experimental results. 相似文献
45.
We report the detection and characterization of the Ni(III) intermediates generated by reaction of (1,4,8,11-tetraazacyclotetradecane)nickel(II) perchlorate with KHSO5. Four Ni(III) intermediates can be trapped or detected through variation in Cl- or KHSO5 concentrations. Upon oxidation of [Ni(cyclam)]2+ by 2.5 equiv of KHSO5, deprotonation of the cyclam ligand generates two red Ni(III) species with lambda max = 530 nm and g perpendicular = 2.20 and g parallel = 2.02 or g perpendicular = 2.16 and g parallel = 2.01 for the axial 4-coordinate or 6-coordinate dichloride species, respectively. These forms decay to Ni(II) products via complex ligand oxidation mechanisms. The Ni(III) dichloride species can be reprotonated and subsequently binds to DNA via an outer-sphere interaction as evidenced by the inverted sign of the CD signal near 400 nm. Cumulatively, the results indicate that the Ni(III) center is coordinately saturated under excess chloride conditions but is still able to interact with DNA substrates. This suggests alternative mechanistic pathways for DNA modification by reaction of [Ni(cyclam)]2+ with KHSO5 and possibly other Ni(II) complexes as well. 相似文献
46.
Mindy I Davis Allen M Orville Frank Neese Jeffrey M Zaleski John D Lipscomb Edward I Solomon 《Journal of the American Chemical Society》2002,124(4):602-614
The geometric and electronic structure of the high-spin ferric active site of protocatechuate 3,4-dioxygenase (3,4-PCD) has been examined by absorption (Abs), circular dichroism (CD), magnetic CD (MCD), and variable-temperature-variable-field (VTVH) MCD spectroscopies. Density functional (DFT) and INDO/S-CI molecular orbital calculations provide complementary insight into the electronic structure of 3,4-PCD and allow an experimentally calibrated bonding scheme to be developed. Abs, CD, and MCD indicate that there are at least seven transitions below 35 000 cm(-1) which arise from tyrosinate ligand-to-metal-charge transfer (LMCT) transitions. VTVH MCD spectroscopy gives the polarizations of these LMCT bands in the principal axis system of the D-tensor, which is oriented relative to the molecular structure from the INDO/S-CI calculations. Three transitions are associated with the equatorial tyrosinate and four with the axial tyrosinate. This large number of transitions per tyrosinate is due to the pi and importantly the sigma overlap of the two tyrosinate valence orbitals with the metal d orbitals and is governed by the Fe-O-C angle and the Fe-O-C-C dihedral angles. The previously reported crystal structure indicates that the Fe-O-C angles are 133 degrees and 148 degrees for the equatorial and axial tyrosinate, respectively. Each tyrosinate has transitions at different energies with different intensities, which correlate with differences in geometry that reflect pseudo-sigma bonding to the Fe(III) and relate to reactivity. These factors reflect the metal-ligand bond strength and indicate that the axial tyrosinate-Fe(III) bond is weaker than the equatorial tyrosinate-Fe(III) bond. Furthermore, it is found that the differences in geometry, and hence electronic structure, are imposed by the protein. The consequences to catalysis are significant because the axial tyrosinate has been shown to dissociate upon substrate binding and the equatorial tyrosinate in the enzyme-substrate complex is thought to influence asymmetric binding of the chelated substrate moiety via a strong trans influence which activates the substrate for reaction with O2. 相似文献
47.
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49.
V.I. Nizhankovskii A.I. Khar'kovskii A.J. Zaleski 《The European Physical Journal B - Condensed Matter and Complex Systems》1999,10(4):761-766
Spontaneous magnetisation of (100) and (010) surfaces of single crystal MnF2 in the antiferromagnetic state has been discovered. The sign of the surface magnetisation is determined by the difference
in dielectric constants of MnF2 and ambient matter: magnetisation is directed to the substance with smaller .
Received 28 August 1998 and Received in final form 15 December 1998 相似文献
50.
The mechanism of n-heptane evaporation from mesoporous MCM-41 silica was investigated by positron annihilation lifetime spectroscopy (PALS). Experiments were performed in situ during desorption of hydrocarbon under stepwise lowered pressure. Desorption is a quasicontinuous process that corresponds to emptying various types of free volumes in the silica/n-heptane system, including mesopores. Insight into the kinetics of desorption was derived from the changes of PALS spectra associated with succeeding stages of pore emptying. For the investigated system emptying of pores and formation of bubbles in the n-heptane condensate present in regular pores were found to take place at various bulk saturating vapour pressure of the fluid. 相似文献