Theoretical Studies of Excess Electrons Interacting with Water Clusters and of Water on Graphitic Surfaces

匹兹堡大学的Kenneth Jordan获得了化学理论、模型和计算方法项目的一项奖励，用于研究开发理解水中水合电子和离子的理论方法。这项工作增强了人们对氢键溶剂中多余电子的行为以及弱相互作用对界面上水的性质的作用的理解。许多重要的化学和生物过程，包括电化学过程和光合作用中的电子转移，都是由存在水的多余电子驱动的。尽管对水合电子和附着在水团簇上的多余电子进行了大量的实验和理论研究，但对这些物种的结构和动力学还缺乏全面的了解。Jordan小组正在进行的理论研究采用最先进的电子-水和水-水势来模拟比过去可能的更大尺寸的带负电荷的水团。这项工作还包括两个促进弱相互作用领域知识的项目。其中第一个涉及发展新的方法来修正远距离相互作用的密度泛函理论，而第二个涉及发展描述水单体和石墨表面之间相互作用的精确电位。该项目的最终目标是使用新开发的精确力场在石墨表面和碳纳米管中模拟水。这项工作正在对许多科学领域产生更广泛的影响，通过PI与特柳赖德科学研究中心广泛的教育和推广活动，其影响进一步扩大。

Kenneth Jordan of the University of Pittsburgh is supported by an award from the Chemical Theory, Models and Computational Methods program for research to develop theoretical methods for understanding hydrated electrons and ions in water. The work is producing an enhanced understanding of the behavior of excess electrons in hydrogen-bonding solvents and of the role of weak interactions on the properties of water at interfaces. Many important chemical and biological processes, including electrochemical processes and electron transfer in photosynthesis, are driven by excess electrons in the presence of water. Despite the large number of experimental and theoretical studies of the hydrated electron and of the excess electron attached to water clusters, a comprehensive understanding of the structures and dynamics of these species is lacking. The theoretical studies being carried out by the Jordan group employ state-of-the-art electron-water and water-water potentials to simulate negatively-charged water clusters of a larger size than has been possible in the past. The work also includes two projects that advance knowledge in the area of weak interactions. The first of these involves the development of new methods of correcting density functional theory for long-range interactions, while the second involves the development of accurate potentials describing the interaction between a water monomer and the graphite surface. The ultimate goal of this project is to perform simulations of water on graphite surfaces and confined in carbon nanotubes using the newly developed, accurate force fields. The work is having a broader impact on many fields of science and its impact is further broadened through the PI's extensive educational and outreach activities with the Telluride Science Research Center.