Intramolecular Vibrations Complement the Robustness of Primary Charge Separation in a Dimer Model of the Photosystem II Reaction Center
Intramolecular Vibrations Complement the Robustness of Primary Charge Separation in a Dimer Model of the Photosystem II Reaction Center
复制标题
DOI：
10.1021/acs.jpclett.8b02119
复制
发表时间：
2018-09-06
影响因子：
5.7
通讯作者：
Ishizaki, Akihito
中科院分区：
文献类型：
--
作者：
Fujihashi, Yuta;Higashi, Masahiro;Ishizaki, Akihito
产氧光合作用的能量转换是由光系统II反应中心蛋白质中的初级电荷分离触发的。在这里，我们调查的蛋白质环境和分子内振动的初级电荷分离的光系统II反应中心的影响。这是通过结合凝聚相电子转移的量子动力学理论和量子化学计算来实现的，以评估叶绿素和脱镁叶绿素分子的振动Huang-Rhys因子。我们报告说，个人的振动模式在促进电荷分离中起着次要的作用，相反，在最近的出版物中的讨论。然而，这些小的贡献积累到相当大的影响电荷分离速率，导致亚皮秒电荷分离几乎独立的驱动力和温度。我们建议，分子内的振动补充的鲁棒性的电荷分离的光系统II反应中心对所涉及的电子能量的固有的大静态无序。
The energy conversion of oxygenic photosynthesis is triggered by primary charge separation in proteins at the photosystem II reaction center. Here, we investigate the impacts of the protein environment and intramolecular vibrations on primary charge separation at the photosystem II reaction center. This is accomplished by combining the quantum dynamic theories of condensed phase electron transfer with quantum chemical calculations to evaluate the vibrational Huang-Rhys factors of chlorophyll and pheophytin molecules. We report that individual vibrational modes play a minor role in promoting charge separation, contrary to the discussion in recent publications. Nevertheless, these small contributions accumulate to considerably influence the charge separation rate, resulting in subpicosecond charge separation almost independent of the driving force and temperature. We suggest that the intramolecular vibrations complement the robustness of the charge separation in the photosystem II reaction center against the inherently large static disorder of the involved electronic energies.