Rutkauskas Danielis, Novoderezhkin Vladimir, Cogdell Richard J, van Grondelle Rienk
Department of Biophysics and Physics of Complex Systems, Division of Physics and Astronomy, Faculty of Sciences, Vrije Universiteit, 1081 HV Amsterdam, The Netherlands.
Biophys J. 2005 Jan;88(1):422-35. doi: 10.1529/biophysj.104.048629. Epub 2004 Oct 22.
We have investigated the energy landscape of the bacterial photosynthetic peripheral light-harvesting complex LH2 of purple bacterium Rhodopseudomonas acidophila by monitoring sequences of fluorescence spectra of single LH2 assemblies, at room temperature, with different excitation intensities as well as at elevated temperatures, utilizing a confocal microscope. The fluorescence peak wavelength of individual LH2 complexes was found to abruptly move between long-lived quasi-stable levels differing by up to 30 nm. The frequency and size of these fluorescence peak movements were found to increase linearly with the excitation intensity. These spectral shifts either to the blue or to the red were accompanied by a broadening and decrease of the intensity of the fluorescence spectrum. The probability for a particle to undergo significant spectral shift in either direction was found to be roughly the same. Using the modified Redfield theory, the observed changes in spectral shape and intensity were accounted for by changes in the realization of the static disorder. Long lifetimes of the quasi-stable states suggest large energetic barriers between the states characterized by different emission spectra.
我们利用共聚焦显微镜,通过监测单个嗜酸性红假单胞菌紫色细菌光合外周捕光复合物LH2在室温下、不同激发强度以及高温下的荧光光谱序列,研究了其能量景观。发现单个LH2复合物的荧光峰值波长会在相差高达30 nm的长寿命准稳定水平之间突然移动。这些荧光峰值移动的频率和幅度随激发强度呈线性增加。这些向蓝色或红色的光谱位移伴随着荧光光谱强度的展宽和降低。发现粒子在任一方向上发生显著光谱位移的概率大致相同。使用修正的雷德菲尔德理论,光谱形状和强度的观测变化可由静态无序实现的变化来解释。准稳定态的长寿命表明,具有不同发射光谱的态之间存在较大的能量势垒。