Department of Chemistry, Georgia State University , Atlanta, Georgia 30302, United States.
Chemistry Department, Bowling Green State University , Overman Hall, Bowling Green, Ohio 43403, United States.
Chem Rev. 2017 Nov 22;117(22):13502-13565. doi: 10.1021/acs.chemrev.7b00177. Epub 2017 Oct 30.
Ultrafast processes in light-absorbing proteins have been implicated in the primary step in the light-to-energy conversion and the initialization of photoresponsive biological functions. Theory and computations have played an instrumental role in understanding the molecular mechanism of such processes, as they provide a molecular-level insight of structural and electronic changes at ultrafast time scales that often are very difficult or impossible to obtain from experiments alone. Among theoretical strategies, the application of hybrid quantum mechanics and molecular mechanics (QM/MM) models is an important approach that has reached an evident degree of maturity, resulting in several important contributions to the field. This review presents an overview of state-of-the-art computational studies on subnanosecond events in rhodopsins, photoactive yellow proteins, phytochromes, and some other photoresponsive proteins where photoinduced double-bond isomerization occurs. The review also discusses current limitations that need to be solved in future developments.
在光吸收蛋白中的超快过程被认为是光到能量转换的初始步骤和光响应生物功能的初始化步骤。理论和计算在理解这些过程的分子机制方面发挥了重要作用，因为它们提供了在超快时间尺度上的结构和电子变化的分子水平的见解，而这些变化通常很难或不可能仅从实验中获得。在理论策略中，混合量子力学和分子力学（QM/MM）模型的应用是一种重要的方法，已经达到了明显的成熟程度，为该领域做出了几项重要贡献。本综述介绍了在视紫红质、光激活黄色蛋白、植物色素和其他一些发生光诱导双键异构化的光响应蛋白中，关于亚纳秒事件的最新计算研究的概述。该综述还讨论了未来发展中需要解决的当前限制。
