Cui XueYan, Yan YiJing, Wei JianHua
Department of Physics & Beijing Key Laboratory of Optoelectronic Functional Materials and Micro-nano Devices, Renmin University of China, Beijing 100872, China.
Department of Chemical Physics & Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
J Phys Chem B. 2020 Mar 26;124(12):2354-2362. doi: 10.1021/acs.jpcb.0c00266. Epub 2020 Mar 16.
In recent years, two-dimensional (2D) electronic spectroscopy experiments prove that the excitation energy transfer (EET) in photosynthetic light-harvesting systems presents long-lived electronic quantum beating signals. After being discovered in the light-harvesting system, the quantum coherence effect has aroused widespread discussion. To illustrate the EET process in the Fenna-Matthews-Olson (FMO) and phycocyanin 645 (PC645) complex, the local protein environment is often thought to be the same; however, this is ambivalent to the practical structural analysis of the light-harvesting complex. By adopting the dissipaton equation of motion theory, we present the effect of a heterogeneous protein environment on the energy transfer process with accurate numerical results. We demonstrate that the energy transfer process relies on the local heterogeneous environment for the FMO complex. A similar good agreement is found for the PC645 complex. Furthermore, we discuss the optimal value of different chromophores in the excitation energy transfer process by controlling the environmental characteristics.
近年来，二维（2D）电子光谱实验证明，光合光捕获系统中的激发能量转移（EET）呈现出长寿命的电子量子拍频信号。在光捕获系统中被发现后，量子相干效应引起了广泛讨论。为了阐明费纳-马修斯-奥尔森（FMO）和藻蓝蛋白645（PC645）复合物中的EET过程，局部蛋白质环境通常被认为是相同的；然而，这与光捕获复合物的实际结构分析相矛盾。通过采用运动耗散方程理论，我们给出了异质蛋白质环境对能量转移过程的影响，并得到了精确的数值结果。我们证明，FMO复合物的能量转移过程依赖于局部异质环境。对于PC645复合物也发现了类似的良好一致性。此外，我们通过控制环境特征来讨论激发能量转移过程中不同发色团的最佳值。
