Theoretical and Computational Methods for Long-Distance Electron Tunneling in Biological Systems

在这个由化学部理论和计算化学计划、数学科学部计算数学计划和分子和细胞生物科学部分子生物物理学计划共同资助的项目中，Stuchebrukhov将开发研究生物系统中长距离电子隧穿的理论和计算方法。Stuchebrukhov早些时候开发的隧道电流方法将进一步测试并应用于特定的实验系统。这项工作的重点是改进计算方法，使其适用于计算非常小的隧道相互作用，并纳入由于蛋白质核动力学而产生的非弹性效应。这项工作将研究一些对实验者很重要的问题，例如蛋白质动力学如何影响长距离电子转移的速度，电子转移路径是否真实，以及长距离质子转移与电子转移步骤的耦合问题。这个项目致力于提高计算生物体系中电子转移速率的准确性，这是化学和生物学交界处的一个重要问题。所研究的问题与理解一些重要系统的功能和动力学有关，这些系统的分子结构最近已为人所知，例如光合作用反应中心，从而可以在理论和实验之间进行比较。归根结底，这项工作对于理解如何利用新技术，包括纳米科学和生物技术，以及在培训本科生、研究生和博士后将理论和计算化学应用于当代科学的重要问题方面是有价值的。

In this project funded jointly by the Theoretical and Computational Chemistry Program of the Chemistry Division, the Computational Mathematics Program of the Division of Mathematical Sciences, and the Molecular Biophysics Program in the Division of Molecular and Cellular Biosciences, Stuchebrukhov will develop theoretical and computational methods to study long-distance electron tunneling in biological systems. The Tunneling Currents Method, developed earlier by Stuchebrukhov, will be further tested and applied to specific experimental systems. Among the issues this work will focus on are refining the computational approach to make it useful for calculating very small tunneling interactions and incorporating the inelastic effects that are due to protein nuclear dynamics. The work will examine a number of issues that are important to experimentalists, such as how protein dynamics affect the rates of long-distance electron transfer, whether electron-transfer pathways are real or not, and the problem of coupling proton-transfers with electron transfer steps over long distances. This project focuses on improving the accuracy of calculating electron transfer rates in biological systems, an important problem at the interface of chemistry and biology. The issues examined relate to understanding the function and dynamics of a number of important systems whose molecular structures have recently become known, such as photosynthetic reaction centers, allowing a comparison between theory and experiment. Ultimately this work is valuable in understanding how to utilize new technologies, including nanoscale science and biotechnology, as well as in training undergraduate, graduate, and postdoctoral students in the applications of theoretical and computational chemistry to important problems in contemporary science.