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Uulke A. van der Heide Marc A. M. J. Zandvoort Ernst van Faassen Gijs van Ginkel Yehudi K. Levine 《Journal of fluorescence》1993,3(4):271-279
Measurements of fluorescence depolarization decays are widely used to obtain information about the molecular order and rotational dynamics of fluorescent probe molecules in membrane systems. This information is obtained by least-squares fits of the experimental data to the predictions of physical models for motion. Here we present a critical review of the ways and means of the data analysis and address the question how and why totally different models such as Brownian rotational diffusion and wobble-in-cone provide such convincing fits to the fluorescence anistropy decay curves. We show that while these models are useful for investigating the general trends in the behavior of the probe molecules, they fail to describe the underlying motional processes. We propose to remedy this situation with a model in which the probe molecules undergo fast, though restricted local motions within a slowly rotating cage in the lipid bilayer structure. The cage may be envisaged as a free volume cavity between the lipid molecules, so that its position and orientation change with the internal conformational motions of the lipid chains. This approach may be considered to be a synthesis of the wobble-in-cone and Brownian rotational diffusion models. Importantly, this compound motion model appears to provide a consistent picture of fluorescent probe behavior in both oriented lipid bilayers and lipid vesicle systems. 相似文献
23.
The critical exponent of degenerate parabolic systems 总被引:1,自引:0,他引:1
Yuan-Wei Qi H. A. Levine 《Zeitschrift für Angewandte Mathematik und Physik (ZAMP)》1993,44(2):249-265
The Cauchy problemu
t=u
+v
p
,v
t
=v
+u
q
is studied, wherex R
N
, 0 <t < and ,,p andq, are positive exponents. It is proved that ifp,q 1 and 1 <pq < 1 + 2 max(p + ,q + )/n then every nontrivial non-negative solution is not global in time; whereaspq > 1 + 2 max(p + , q + )/n then there exist both positive global solutions and non-global solutions. In addition, the decaying in time of solutions tou
t,=u
inR
n
× (0, ), an equation which occurs naturally in our study of above systems, is studied and solutions with the fastest decaying in time are constructed. 相似文献
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27.
Water proton chemical shifts have been measured for aqueous solutions of tetrabutylammonium butyrate and tetrabutylammonium bromide as a function of salt concentration and temperature. Large, negative (downfield) salt shifts are reported for Bu4NBut solutions at temperatures below 33°C. The chemical shift becomes more negative with increasing molality up to about 0.5 m: at higher compositions, the chemical shift levels or becomes less negative. These results suggest that hydrophobic hydration cages formed under the influence of Bu4NBut have their maximum size at approximately 0.5 m and that at higher concentrations overlap of these cages must occur as suggested by earlier thermodynamic investigations. The observed downfield molal chemical shifts are much larger than those estimated from individual ionic contributions, suggesting a mutual enhancement or linking together of hydration cages even in dilute solution. 相似文献
28.
The short-time intramolecular dynamics of highly vibrationally excited HCCD and DCCD, as determined by classical trajectories, have qualitative features distinct from HCCH and from one another. The possible differences are also considered from the point of view of the symmetries of the normal modes. The short-time evolution will be reflected in the coarse-grained frequency spectrum and could be detectable via stimulation emission pumping. 相似文献
29.
Ko C Levine B Toniolo A Manohar L Olsen S Werner HJ Martínez TJ 《Journal of the American Chemical Society》2003,125(42):12710-12711
The photoisomerization mechanism of the neutral form of the photoactive yellow protein (PYP) chromophore is investigated using ab initio quantum chemistry and first-principles nonadiabatic molecular dynamics (ab initio multiple spawning or AIMS). We identify the nature of the two lowest-lying excited states, characterize the short-time behavior of molecules excited directly to S2, and explain the origin of the experimentally observed wavelength-dependent photoisomerization quantum yield. 相似文献
30.
Both classical trajectory and quantal scattering calculations indicate that the branching ratio in the F+HD reaction varies considerably with the initial rotational state of HD. Information theory argues that this variation must be reflected in the distribution of the reaction products. Hence, given the (normalized) product distribution for each reaction path one should be able to predict the dependence of the branching ratio on the state of the reagents. The trajectory computations of Muckerman are used to illustrate the procedure. First the dynamic constraint is identified and then the reaction probability matrix is constructed. The determination (“synthesis”) of the matrix, in terms of the given constraint invokes information theory and, in particular, the procedure of maximising the entropy. The branching ratio is readily computed from the elements of the probability matrix. Very good agreement is obtained between the trajectory-computed and the synthetic branching ratio for all initial rotational states of HD.The F+HD reaction has three possible final arrangement channels (one nonreactive and two reactive ones) and is used to illustrate the structure of the reaction probability matrix and the associated entropy measures. 相似文献