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921.
André Luiz Tessaro Vagner Roberto Batistela Augusto César Gracetto Hueder Paulo Moisés de Oliveira Rosana Lazara Sernaglia Vagner Roberto de Souza Wilker Caetano Noboru Hioka 《Journal of Physical Organic Chemistry》2011,24(2):155-161
Benzoporphyrin monoacid derivatives, here named B3A and B3B, are promising new drugs for photodynamic therapy. Although both isomers show interesting characteristics as photosensitizing compounds, they have some distinct physicochemical properties such as the tendency to self‐aggregate in water‐rich media. Because pH drives the presence of each species, the pKa of these compounds assumes strategic importance. However, traditional micro‐titration methods and UV–Vis absorption techniques fail to give reliable pKa values due to the characteristics of this highly complex system, such as the precipitation of hydrophobic species, close pKa values, and high absorption band superposition. In the present work, chemometric tools are employed to evaluate pKa, and the kinetic tendency of monomers to undergo self‐aggregation is investigated. In solvent mixtures at low water percentage in ethanol, both B3A and B3B are stabilized in a monomeric state. However, in mixtures with a high water content, self‐aggregation takes place, mainly under a mild pH acid condition (3 < pH < 6), in which the prevalent protolytic species of both isomers is the neutral charged form, compounds with carboxylic and porphyrin free‐base groups. It is demonstrated that both isomers can undergo aggregation following a self‐catalytic mechanism, which is 2000 times slower to B3A than B3B. For B3A, the aggregation is manifested by a decrease in the monomer band with the aggregation band probably superposed to that of the monomer. For B3B, together with the decrease in the monomer band, a new band related to self‐aggregates is observed. Copyright © 2010 John Wiley & Sons, Ltd. 相似文献
922.
Bagrat A. Shainyan Elena N. Suslova Erich Kleinpeter 《Journal of Physical Organic Chemistry》2011,24(12):1188-1192
4,4‐Dimethyl‐4‐silathiane and its S‐oxides [n = 0 ( 1 ), 1 ( 2 ), 2 ( 3 )] were studied experimentally by variable temperature dynamic NMR spectroscopy down to 103 K and the frozen ring inversion was revealed for all three compounds. The barriers for the degenerate ring inversion in 1 and 3 were measured to be 4.8 and 5.0 kcal/mol at the coalescence temperatures of 111 and 116 K, respectively, and practically coincide with the calculated barriers of 4.60 kcal/mol in 1 and 4.46 kcal/mol in 3 . The frozen equilibrium mixture 2‐ax/2‐eq contains 37% of the 2‐ax and 63% of the 2‐eq conformer. The ring inversion barrier proved to be ca. 4.8 kcal/mol. Calculations at the B3LYP/6‐311+G(d,p) level of theory showed the 2‐ax conformer to be 0.90 kcal/mol more stable than the 2‐eq conformer in the gas phase whereas in solution the relative stability of the conformers calculated using the PCM model at the same level of theory is inverted to become 0.19 (in CHCl3) or 0.36 kcal/mol (in DMSO) in favor of the 2‐eq conformer. The chair–chair interconversion mechanism of sulfoxide 2 includes two intermediate energetically equivalent 1,4‐twist forms and the 2,5‐boat transition state: 2‐ax (chair) ? 2 (1,4‐twist) ? [ 2 (2,5‐boat)]≠ ? 2 (1,4‐twist) ? 2‐eq (chair). The calculated ring inversion barriers are 5.1 ( 2‐ax → 2‐eq ) and 4.2 kcal/mol ( 2‐eq → 2‐ax ) in the gas phase, and 4.03 and 4.22 kcal/mol, respectively, in chloroform. Copyright © 2011 John Wiley & Sons, Ltd. 相似文献
923.
Dynamic bifurcation of a modified Kuramotoben Sivashinsky equation with higher-order nonlinearity
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Under the periodic boundary condition, dynamic bifurcation and stability in the modified Kuramoto—Sivashinsky equation with a higher-order nonlinearity μ(ux)puxx are investigated by using the centre manifold reduction procedure. The result shows that as the control parameter crosses a critical value, the system undergoes a bifurcation from the trivial solution to produce a cycle consisting of locally asymptotically stable equilibrium points. Furthermore, for cases in which the distances to the bifurcation points are small enough, one-order approximations to the bifurcation solutions are obtained. 相似文献
924.
925.
926.
927.
We present two continuous symmetry reduction methods for reducing high-dimensional dissipative flows to local return maps. In the Hilbert polynomial basis approach, the equivariant dynamics is rewritten in terms of invariant coordinates. In the method of moving frames (or method of slices) the state space is sliced locally in such a way that each group orbit of symmetry-equivalent points is represented by a single point. In either approach, numerical computations can be performed in the original state space representation, and the solutions are then projected onto the symmetry-reduced state space. The two methods are illustrated by reduction of the complex Lorenz system, a five-dimensional dissipative flow with rotational symmetry. While the Hilbert polynomial basis approach appears unfeasible for high-dimensional flows, symmetry reduction by the method of moving frames offers hope. 相似文献
928.
929.
We revisit the problem of quantizing field theories on noncommutative Moyal space–time with light-like noncommutativity. To tackle the issues arising from noncommuting and hence nonlocal time, we argue that for this case light-front quantization procedure should be employed. In this appropriate quantization scheme we perform the non-planar loop analysis for the light-like noncommutative field theories. One of the important and peculiar features of light-front quantization is that the UV cutoff of the light-cone Hamiltonian manifests itself as an IR cutoff for the light-cone momentum, p+. Due to this feature, the naive results of covariant quantization for the light-like case allude to the absence of the UV/IR mixing in the light-front quantization. However, by a careful analysis of non-planar loop integrals we show that this is not the case and the UV/IR mixing persists. In addition, we argue in favour of the perturbative unitarity of light-like noncommutative field theories in the light-front quantization scheme. 相似文献
930.
Nicoleta ALDEA Gheorghe MUNTEANU 《数学物理学报(B辑英文版)》2014,(4):995-1011
In this paper we extend the results obtained in [3], where are investigated the general settings of the two-dimensional complex Finsler manifolds, with respect to a local complex Berwald frame. The geometry of such manifolds is controlled by three real invariants which live on T ′M : two horizontal curvature invariants K and W and one vertical curvature invariant I. By means of these invariants are defined both the horizontal and the vertical holomorphic sectional curvatures. The complex Landsberg and Berwald spaces are of particular interest. Complex Berwald spaces coincide with K¨ahler spaces, in the two-dimensional case. We establish the necessary and sufficient condition under which K is a constant and we obtain a characterization for the K¨ahler purely Hermitian spaces by the fact K = W = constant and I = 0. For the class of complex Berwald spaces we have K = W = 0.Finally, a classification of two-dimensional complex Finsler spaces for which the horizontal curvature satisfies a special property is obtained. 相似文献