Department of Nanoscience, Madrid Institute for Advanced Studies, 28049 Cantoblanco, Spain.
Proc Natl Acad Sci U S A. 2012 Jan 31;109(5):1473-8. doi: 10.1073/pnas.1113080109. Epub 2012 Jan 23.
Energy transfer (ET) between B850 and B875 molecules in light harvesting complexes LH2 and LH1/RC (reaction center) complexes has been investigated in membranes of Rhodopseudomonas palustris grown under high- and low-light conditions. In these bacteria, illumination intensity during growth strongly affects the type of LH2 complexes synthesized, their optical spectra, and their amount of energetic disorder. We used a specially built femtosecond spectrometer, combining tunable narrowband pump with broadband white-light probe pulses, together with an analytical method based on derivative spectroscopy for disentangling the congested transient absorption spectra of LH1 and LH2 complexes. This procedure allows real-time tracking of the forward (LH2 → LH1) and backward (LH2←LH1) ET processes and unambiguous determination of the corresponding rate constants. In low-light grown samples, we measured lower ET rates in both directions with respect to high-light ones, which is explained by reduced spectral overlap between B850 and B875 due to partial redistribution of oscillator strength into a higher energetic exciton transition. We find that the low-light adaptation in R. palustris leads to a reduced elementary backward ET rate, in accordance with the low probability of two simultaneous excitations reaching the same LH1/RC complex under weak illumination. Our study suggests that backward ET is not just an inevitable consequence of vectorial ET with small energetic offsets, but is in fact actively managed by photosynthetic bacteria.
在高光和低光条件下生长的沼泽红假单胞菌的膜中,研究了聚光复合物 LH2 和 LH1/RC(反应中心)复合物中 B850 和 B875 分子之间的能量转移(ET)。在这些细菌中,生长期间的光照强度强烈影响合成的 LH2 复合物的类型、它们的光学光谱以及它们的能量无序程度。我们使用了一种专门构建的飞秒光谱仪,将可调谐窄带泵与宽带白光探测脉冲相结合,同时使用基于导数光谱学的分析方法来解卷积 LH1 和 LH2 复合物的拥挤瞬态吸收光谱。该程序允许实时跟踪向前(LH2→LH1)和向后(LH2←LH1)ET 过程,并明确确定相应的速率常数。在低光生长的样品中,我们测量到两个方向的 ET 速率都低于高光生长的样品,这可以解释为由于振子强度部分重新分配到更高能量的激子跃迁,B850 和 B875 之间的光谱重叠减少。我们发现,沼泽红假单胞菌的低光适应导致基本的向后 ET 速率降低,这与弱光照下两个同时激发到达相同 LH1/RC 复合物的概率较低相符。我们的研究表明,向后 ET 不仅仅是具有小能量偏移的矢量 ET 的必然结果,实际上是由光合细菌主动管理的。