Computational Studies of Nonequilibrium processes in Electrochemical Materials Science

技术概述：该奖项支持在电化学材料科学中非平衡现象的计算和理论研究方面的研究和教育。这些研究涉及特定实验系统的建模，对这些系统重要的基本非平衡现象的调查，以及计算和理论方法的进一步发展。将与实验小组合作研究的特殊实验现象是单晶金表面的电化学脉冲电位研究中的岛屿生长和溶解，以及验证由PI的计算机模拟提出的研究电极表面动力学的新方法。研究的特殊非平衡现象包括电化学金属沉积和非均相催化反应中横向扩散的影响，以及由振荡力驱动远离平衡的系统中的滞后。所提出的研究将使用的主要方法是模型系统的大规模计算机仿真。将使用连续和离散模型，计算方法将包括动力学蒙特卡罗（KMC）模拟和随机微分方程的数值解，两者都使用从量子力学密度泛函理论计算中获得的模型参数。模拟数据将使用几种理论方法进行分析，包括有限尺寸缩放理论，随机过程理论和统计学。该研究具有更广泛的影响，超出了所进行的特定科学调查，广泛地有助于理解非平衡过程的问题，与技术发展有关，并具有教育效益。由于自然界和技术中所有与时间有关的现象根据定义都是非平衡的，因此非平衡统计力学是一个重要的研究领域。这项研究增加了我们对非平衡过程的基本理解。更具体地说，这项研究提高了对电极-电解质界面非平衡过程的理解，从而有助于未来发展新的、基于电化学的先进纳米材料制造工艺。通过研究开发的这些基础知识和仿真算法可以应用于许多科技领域，包括材料科学、化学、生物学，甚至通信网络和电网的设计和分析。这种计算密集型的研究对于在发现过程中涉及各个层次的学徒来说是理想的。它将为各级教育做出贡献，同时通过让本科生、研究生和博士后参与进来，包括女性和少数族裔，他们将指导K-12学生。研究结果将通过各种专业期刊上的文章、科学会议上的演讲、面向公众的介绍以及万维网进行传播。非技术概述：该奖项支持理论和计算研究，以及通过电化学方法在纳米尺度（约为千万分之一英寸）上生长材料和原子结构的教育。在过去的二十年里，实验技术的发展使得电化学方法能够制造出从纳米尺度结构中获得功能的高科技材料。这些方法正迅速成为传统方法的成本效益替代品。这些令人印象深刻的实验发展与计算机技术和计算方法的惊人进步相匹配。PI将使用计算机模拟方法来研究纳米结构是如何在电极材料表面生长的，电极材料浸泡在有电流流过的化学溶液中。对这些增长现象的研究促进了对本质上不平衡现象的理解，这是现代统计物理学中一个非常感兴趣的领域。由于自然界和技术中所有与时间有关的现象根据定义都是非平衡的，因此非平衡统计力学是一项必不可少的研究。这种计算密集型的研究对于在发现过程中涉及各个层次的学徒来说是理想的。它将为各级教育做出贡献，同时通过让本科生、研究生和博士后参与进来，包括女性和少数族裔，他们将指导K-12学生。研究结果将通过各种专业期刊上的文章、科学会议上的演讲、面向公众的介绍以及万维网进行传播。

TECHNICAL SUMMARY:This award supports research and education in computational and theoretical studies of nonequilibrium phenomena in electrochemical materials science. These studies are concerned with modeling of specific experimental systems, with investigation of fundamental nonequilibrium phenomena of importance to such systems, and with further development of computational and theoretical methods.The particular experimental phenomena, which will be investigated in collaboration with experimental groups, are island growth and dissolution in electrochemical pulsed-potential studies of single-crystal gold surfaces, and verification of a new method to study the dynamics of electrode surfaces that was suggested by the PI's computer simulations. Particular nonequilibrium phenomena that are investigated include the influence of lateral diffusion during electrochemical metal deposition and in heterogeneous catalytic reactions, and hysteresis in systems that are driven far from equilibrium by an oscillating force.The main method that will be used in the proposed research is large-scale computer simulation of model systems. Both continuous and discrete models will be used, and the computational methods will include kinetic Monte Carlo (KMC) simulations and numerical solution of stochastic differential equations, both with model parameters obtained from quantum-mechanical density-functional-theory calculations. The simulation data will be analyzed using several theoretical methods, including finite-size scaling theory, theory of stochastic processes, and statistics.The research has broader impact beyond the particular scientific investigations undertaken and contributes broadly to understanding issues of nonequilibrium processes and is relevant to technological development and has educational benefits. Since all time-dependent phenomena in nature, as well as in technology, are out of equilibrium by definition, nonequilibrium statistical mechanics is an essential research area. This research adds to our fundamental understanding of nonequilibrium processes. More specifically, this research improves understanding of nonequilibrium processes at electrode-electrolyte interfaces, and thereby contributes to the future development of new, electrochemistry-based manufacturing processes for advanced nanomaterials. Such fundamental knowledge and simulation algorithms developed through the research are applicable in many scientific and technological fields, including materials science, chemistry, biology, and even to the design and analysis of communications networks and power grids. This computationally intensive research is ideal for involving apprentices at all levels in the discovery process. It will contribute to education at all levels while including women and minorities by involving undergraduate and graduate students and postdoctoral fellows, who will mentor K-12 students. The results of the research will be communicated through articles in a wide spectrum of professional journals, through talks at scientific meetings, and through presentations for the general public, as well as through the World Wide Web.NONTECHNICAL SUMMARY:This award supports theoretical and computational research, and education on the growth of materials and structures of atoms on the scale of nanometers, about one ten-millionth of an inch, by electrochemical methods. During the last two decades experimental techniques have become available that enable electrochemical methods to manufacture high-tech materials that derive their functionality from structure on the nanometer scale. These methods are rapidly becoming cost-effective alternatives to traditional methods. These impressive experimental developments are matched by spectacular progress in computer technology and computational methods. The PI will use computer simulation methods to study how nanoscale structures grow on the surface of electrode materials immersed in a chemical solution with an electric current flowing through the electrodes. The study of growth phenomena like these advances the understanding of phenomena that are intrinsically out of equilibrium, an area of intense interest in modern statistical physics. Since all time-dependent phenomena in nature, as well as in technology, are out of equilibrium by definition, nonequilibrium statistical mechanics is an essential research.This computationally intensive research is ideal for involving apprentices at all levels in the discovery process. It will contribute to education at all levels while including women and minorities by involving undergraduate and graduate students and postdoctoral fellows, who will mentor K-12 students. The results of the research will be communicated through articles in a wide spectrum of professional journals, through talks at scientific meetings, and through presentations for the general public, as well as through the World Wide Web.