Faculty of Biomedical and Life Sciences, University of Glasgow, Glasgow, United Kingdom.
Biophys J. 2009 Dec 2;97(11):3019-28. doi: 10.1016/j.bpj.2009.09.023.
Energy transfer processes in photosynthetic light harvesting 2 (LH2) complexes isolated from purple bacterium Rhodopseudomonas palustris grown at different light intensities were studied by ground state and transient absorption spectroscopy. The decomposition of ground state absorption spectra shows contributions from B800 and B850 bacteriochlorophyll (BChl) a rings, the latter component splitting into a low energy and a high energy band in samples grown under low light (LL) conditions. A spectral analysis reveals strong inhomogeneity of the B850 excitons in the LL samples that is well reproduced by an exponential-type distribution. Transient spectra show a bleach of both the low energy and high energy bands, together with the respective blue-shifted exciton-to-biexciton transitions. The different spectral evolutions were analyzed by a global fitting procedure. Energy transfer from B800 to B850 occurs in a mono-exponential process and the rate of this process is only slightly reduced in LL compared to high light samples. In LL samples, spectral relaxation of the B850 exciton follows strongly nonexponential kinetics that can be described by a reduction of the bleach of the high energy excitonic component and a red-shift of the low energetic one. We explain these spectral changes by picosecond exciton relaxation caused by a small coupling parameter of the excitonic splitting of the BChl a molecules to the surrounding bath. The splitting of exciton energy into two excitonic bands in LL complex is most probably caused by heterogenous composition of LH2 apoproteins that gives some of the BChls in the B850 ring B820-like site energies, and causes a disorder in LH2 structure.
在不同光照强度下生长的紫色细菌 Rhodopseudomonas palustris 中分离出的光合光捕获 2(LH2)复合物的能量转移过程通过基态和瞬态吸收光谱进行了研究。基态吸收光谱的分解表明 B800 和 B850 细菌叶绿素(BChl)a 环的贡献,后一组分在低光(LL)条件下生长的样品中分裂成低能和高能带。光谱分析表明,LL 样品中的 B850 激子存在强烈的不均匀性,这可以通过指数型分布很好地再现。瞬态光谱显示低能和高能带的漂白,以及各自的蓝移激子-双激子跃迁。不同的光谱演化通过全局拟合程序进行了分析。B800 到 B850 的能量转移发生在单指数过程中,与高光样品相比,该过程的速率在 LL 中仅略有降低。在 LL 样品中,B850 激子的光谱弛豫遵循强烈的非指数动力学,可以通过高能激子成分的漂白减少和低能的红移来描述。我们通过 picosecond 激子弛豫来解释这些光谱变化,这种弛豫是由 BChl a 分子的激子分裂与周围溶剂的小耦合参数引起的。在 LL 复合物中,激子能量分裂成两个激子带最可能是由于 LH2 脱辅基蛋白的异质组成引起的,该组成赋予 B850 环中的一些 BChls B820 样的位能,并导致 LH2 结构的无序。