Fluorescence quenching in model membranes: phospholipid acyl chain distributions around small fluorophores.
Fluorescence quenching in model membranes: phospholipid acyl chain distributions around small fluorophores.
复制标题
模型膜中的荧光猝灭:小荧光团周围的磷脂酰基链分布。
DOI:
10.1021/bi00470a018
复制
发表时间:
1990
期刊:
影响因子:
2.9
通讯作者:
Feigenson,GW
中科院分区:
文献类型:
--
作者:
Yeager,MD;Feigenson,GW
Mark D. Yeager1 and Gerald W. Feigenson** Section of Biochemistry, Molecular and Cell Biology, Cornell University, Ithaca, New York 14853 Received August 7, 1989; Revised Manuscript Received December 20, 1989 abstract: Fluorescence quenching in lipid bilayers is treated by a new approach based on calculation of the probability distribution of quenching and nonquenching acyl chains around a fluorophore. The effect of acyl lattice site dependence (ie, correlations of phospholipid sister chain occupancy of neighbor sites) was modeled by use of Monte Carlo simulations of acyl chain occupancy. This explicit accounting of site occupancy correlation was found to fit observed quenching behavior better than did a model wherein phospholipid quenchers are considered to be independent. A key aspect of this approach is to evaluate the rate for quenching in a bilayer composed of pure quenching lipid. In order to evaluate this quenching rate, and also to provide a strong test of the calculated probability distributions, we synthesized lipidswith both acyl chains labeled with a quenching moiety (Br or nitroxide), as well as the more usual single-chain quenchers. The fluorescence of tryptophan octyl ester (TOE), and of the 1, 6-diphenyl-1, 3, 5-hexatriene (DPH) derivatives trimethylammonium-DPH (TMA-DPH) and l-lauroyl-2-(DPH-propionyl) phosphatidylcholine (DPH-PC), was examined. We obtained consistent results with all the fluorophores and quenchers indicating that up to 18 neighboring acyl sites can contribute to quenching, corresponding to twoshells of acyl sites on a hexagonal lattice. Calculated discrete distributions of fluorescence intensities were converted into fluorescence lifetimes and compared with Gaussian and Lorentzian continuous lifetime distributions. Thefluorescence quenching theory presented here may be used to explainquantitatively the heterogeneity of fluorophore environments in multicomponent membranes.