Title: Hidden Vibronic and Excitonic Structure and Vibronic Coherence Transfer in the Bacterial Reaction Center Show Chinese title

Title: 细菌反应中心中的隐含振动和激子结构以及振动相干传递

Abstract: We report two-dimensional electronic spectroscopy (2DES) experiments on the bacterial reaction center (BRC) from purple bacteria, revealing hidden excitonic and vibronic structure. Through analysis of the coherent dynamics of the BRC we resolve specific coherent signatures that allow us to definitively assign the upper exciton energy of the "special pair." This assignment is supported by simulations of coherent dynamics of a reduced excitonic model of the BRC. The simulations also identify nonsecular vibronic coherence transfer processes neglected in standard models of photosynthetic energy transfer and charge separation. In addition, the coherent dynamics reveal multiple quasi-resonances between key intramolecular pigment vibrations and excited state energy gaps in the BRC. The functional significance of such electronic-vibrational resonances for photosynthetic energy transfer and charge separation remains an open question. Show Chinese abstract

Abstract: 我们报告了对紫色细菌的细菌反应中心（BRC）进行的二维电子光谱（2DES）实验，揭示了隐藏的激子和振动结构。 通过分析BRC的相干动力学，我们确定了特定的相干特征，使我们能够明确地分配“特殊对”的上激子能级。 这一分配得到了对BRC简化的激子模型的相干动力学模拟的支持。 模拟还识别出在标准光合能量转移和电荷分离模型中被忽略的非马尔可夫振动相干传递过程。 此外，相干动力学揭示了BRC中关键分子内色素振动与激发态能隙之间的多重准共振。 这种电子-振动共振在光合能量转移和电荷分离中的功能意义仍然是一个开放问题。