Theory of Excitonic Delocalization for Robust Vibronic Dynamics in LH2,The Journal of Physical Chemistry Letters

当前位置： X-MOL 学术 › J. Phys. Chem. Lett. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Theory of Excitonic Delocalization for Robust Vibronic Dynamics in LH2
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-06-04 00:00:00 , DOI: 10.1021/acs.jpclett.8b00933
Felipe Caycedo-Soler ₁ , James Lim ₁ , Santiago Oviedo-Casado ₂ , Niek F. van Hulst _{3,

4} , Susana F. Huelga ₁ , Martin B. Plenio ₁

Affiliation

Nonlinear spectroscopy has revealed long-lasting oscillations in the optical response of a variety of photosynthetic complexes. Different theoretical models that involve the coherent coupling of electronic (excitonic) or electronic–vibrational (vibronic) degrees of freedom have been put forward to explain these observations. The ensuing debate concerning the relevance of either mechanism may have obscured their complementarity. To illustrate this balance, we quantify how the excitonic delocalization in the LH2 unit of Rhodopseudomonas acidophila purple bacterium leads to correlations of excitonic energy fluctuations, relevant coherent vibronic coupling, and importantly, a decrease in the excitonic dephasing rates. Combining these effects, we identify a feasible origin for the long-lasting oscillations observed in fluorescent traces from time-delayed two-pulse single-molecule experiments performed on this photosynthetic complex and use this approach to discuss the role of this complementarity in other photosynthetic systems.

中文翻译：

LH2的稳健振动动力学的激子离域理论

非线性光谱学已经揭示了各种光合配合物的光学响应中的持久振荡。提出了涉及电子（激子）自由度或电子-振动（振动）自由度的相干耦合的不同理论模型来解释这些观察结果。随后关于这两种机制的相关性的辩论可能掩盖了它们的互补性。为了说明这种平衡，我们量化了嗜酸红假单胞菌LH2单元中的激子离域紫色细菌会导致激子能量波动，相关的相干振子耦合，以及重要的是激子移相速率降低。结合这些影响，我们确定了在此光合复合物上进行的延时两脉冲单分子实验中荧光迹线中观察到的长时间振荡的可行起源，并使用这种方法来讨论这种互补性在其他光合系统中的作用。

更新日期：2018-06-04

点击分享查看原文

点击收藏

公开下载

阅读更多本刊最新论文本刊介绍/投稿指南11