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嗜酸性红假单胞菌单个捕光2复合物B850波段的光谱学。I. 实验与蒙特卡洛模拟

Spectroscopy on the B850 band of individual light-harvesting 2 complexes of Rhodopseudomonas acidophila. I. Experiments and Monte Carlo simulations.

作者信息

Ketelaars M, van Oijen A M, Matsushita M, Köhler J, Schmidt J, Aartsma T J

机构信息

Department of Biophysics, Huygens Laboratory, Leiden University, 2300 RA Leiden, The Netherlands.

出版信息

Biophys J. 2001 Mar;80(3):1591-603. doi: 10.1016/S0006-3495(01)76132-2.

Abstract

The electronic structure of the circular aggregate of 18 bacteriochlorophyll a (BChl a) molecules responsible for the B850 absorption band of the light-harvesting 2 (LH2) complex of the photosynthetic purple bacterium Rhodopseudomonas acidophila has been studied by measuring fluorescence-excitation spectra of individual complexes at 1.2 K. The spectra reveal several well-resolved bands that are obscured in the single, broad B850 band observed in conventional absorption measurements on bulk samples. They are interpreted consistently in terms of the exciton model for the circular aggregate of BChl a molecules. From the energy separation between the different exciton transitions a reliable value of the intermolecular interaction is obtained. The spectra of the individual complexes allow for a distinction between the intra- and the intercomplex disorder. In addition to the random disorder, a regular modulation of the interaction has to be assumed to account for all the features of the observed spectra. This modulation has a C(2) symmetry, which strongly suggests a structural deformation of the ring into an ellipse.

摘要

通过测量光合紫色细菌嗜酸红假单胞菌光捕获2(LH2)复合物中负责B850吸收带的18个细菌叶绿素a(BChl a)分子的圆形聚集体的电子结构,在1.2 K下对单个复合物的荧光激发光谱进行了研究。光谱揭示了几个分辨率良好的谱带,这些谱带在对大量样品进行的常规吸收测量中观察到的单一宽B850谱带中被掩盖。根据BChl a分子圆形聚集体的激子模型,对它们进行了一致的解释。从不同激子跃迁之间的能量分离中,获得了分子间相互作用的可靠值。单个复合物的光谱允许区分复合物内部和复合物之间的无序。除了随机无序之外,还必须假设相互作用的规则调制来解释观察到的光谱的所有特征。这种调制具有C(2)对称性,这强烈表明环结构变形为椭圆形。

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