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首页> 外文期刊>The Journal of Chemical Physics >Excitonic energy transfer in light-harvesting complexes in purple bacteria
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Excitonic energy transfer in light-harvesting complexes in purple bacteria

机译:紫色细菌捕光复合物中的激子能量转移

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Two distinct approaches, the Frenkel-Dirac time-dependent variation and the Haken-Strobl model, are adopted to study energy transfer dynamics in single-ring and double-ring light-harvesting (LH) systems in purple bacteria. It is found that the inclusion of long-range dipolar interactions in the two methods results in significant increase in intra- or inter-ring exciton transfer efficiency. The dependence of exciton transfer efficiency on trapping positions on single rings of LH2 (B850) and LH1 is similar to that in toy models with nearest-neighbor coupling only. However, owing to the symmetry breaking caused by the dimerization of BChls and dipolar couplings, such dependence has been largely suppressed. In the studies of coupled-ring systems, both methods reveal an interesting role of dipolar interactions in increasing energy transfer efficiency by introducing multiple intra/inter-ring transfer paths. Importantly, the time scale (4 ps) of inter-ring exciton transfer obtained from polaron dynamics is in good agreement with previous studies. In a double-ring LH2 system, non-nearest neighbor interactions can induce symmetry breaking, which leads to global and local minima of the average trapping time in the presence of a non-zero dephasing rate, suggesting that environment dephasing helps preserve quantum coherent energy transfer when the perfect circular symmetry in the hypothetic system is broken. This study reveals that dipolar coupling between chromophores may play an important role in the high energy transfer efficiency in the LH systems of purple bacteria and many other natural photosynthetic systems.
机译:Frenkel-Dirac随时间变化和Haken-Strobl模型是两种不同的方法,用于研究紫色细菌中单环和双环光收集(LH)系统中的能量传递动力学。发现在两种方法中包含长距离偶极相互作用会导致环内或环间激子转移效率的显着提高。激子传递效率对LH2(B850)和LH1单环上俘获位置的依赖性与仅具有最近邻居耦合的玩具模型中的类似。然而,由于BChls的二聚化和偶极偶合引起的对称性破坏,这种依赖性已被大大抑制。在耦合环系统的研究中,两种方法都通过引入多个环内/环间传输路径,揭示了偶极相互作用在提高能量传输效率方面的有趣作用。重要的是,从极化子动力学获得的环间激子转移的时间尺度(4 ps)与以前的研究非常吻合。在双环LH2系统中,非近邻相互作用会引起对称性破坏,从而在存在非零移相速率的情况下导致平均和平均捕获时间的最小值,这表明环境相移有助于保存量子相干能当假设系统中的完美圆形对称性破裂时,转移。这项研究表明,生色团之间的偶极耦合可能在紫色细菌的LH系统和许多其他自然光合作用系统的高能量转移效率中起重要作用。

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