Theoretical and Computational Studies of Multiple Charge Transfer Reactions in the Condensed Phase

Sharon Hammes-Schiffer由理论和计算化学计划支持，以研究多个电荷转移反应，包括多个质子转移和质子耦合电子转移。 这个项目的主要目标是阐明凝聚相中多重电荷转移反应的基本原理。 为实现这一目标，将采取两种相辅相成的办法。 在第一种方法中，使用混合量子/经典分子动力学方法，溶剂被表示为经典处理的明确分子，而转移质子和活性电子被量子力学处理。 第二种方法基于多态连续介质理论，将溶剂描述为介电连续介质，并对迁移的质子和活性电子进行量子力学处理。 这两种方法将开发和测试的应用程序模型systems.This理论和计算方法的发展和随后的化学和生物相关的系统的应用程序相结合，将提供深入了解多个电荷转移反应的基本原理。 这些反应在质子线（质子沿着沿着水分子链传输）、不对称盐桥和对新陈代谢至关重要的酶反应中很重要。

Sharon Hammes-Schiffer is supported by the Theoretical and Computational Chemistry Program to pursue investigations of multiple charge transfer reactions, including multiple proton transfer and proton-coupled electron transfer. The broad goal of this project is to elucidate the fundamental principles of multiple charge transfer reactions in the condensed phase. Two complementary approaches will be implemented to accomplish this goal. In the first approach, using mixed quantum/classical molecular dynamics methods, the solvent is represented as explicit molecules treated classically, while transferring protons and active electrons are treated quantum mechanically. In the second approach, based on multistate continuum theory, the solvent is represented as a dielectric continuum and the transferring protons and active electrons are treated quantum mechanically. Both approaches will be developed and tested by applications to model systems.This combination of the development of theoretical and computational methodology and subsequent application to chemically and biologically relevant systems will provide insight into the fundamental principles of multiple charge transfer reactions. Such reactions are important in proton wires (proton transport along chains of water molecules), asymmetric salt bridges, and enzyme reactions vital to metabolism.