CAREER: Modeling Metal-Metal Oxide Interactions Using Spherosiloxane Adsorption on Single Crystal Metal Surfaces

结合使用从头计算化学和实验光谱学在解决工程问题正在成为一个越来越普遍的方法。 这个职业生涯项目将强调理论和实验的结合，无论是在执行基础研究，并在教育学生与不同层次的经验。 研究部分的重点是开发一个新的模型系统，这将使详细调查的化学和物理的金属-绝缘体界面。这些界面对于微电子工程、多相催化和化学传感等一系列应用都很重要，但很难用实验或理论来研究，因为它们通常被“埋”在连续的固体层下。 在这个项目中，模型接口，可访问的实验和理论技术将形成的SiO2-like spherosiloxane簇催化金属单晶表面上的吸附。 一组实验技术将用于表征球形硅氧烷的吸附和反应，改变金属基材的组成和形态沿着球形硅氧烷簇的大小。 第一原理计算的结果将用于解释实验观察，有助于理解形成的界面的分子水平结构。 一旦表征，模型界面将用于研究一个重要应用的机制：使用金属氧化物半导体器件检测H2气体。 参与本研究的研究生和本科生团队将获得理论原理、先进光谱技术和实际应用方面的广泛经验。在教学活动中也将强调理论、光谱技术和应用开发的协同作用。 在这些努力中，我们将利用计算化学软件的效用，帮助学生在分子尺度上可视化化学反应。 一个新的研究生/高级本科课程将侧重于分析化学反应过程中的分子尺度转换，与学生的计算化学软件的使用代表课程的一个关键组成部分。 分子建模模拟也将在本科课程中引入更基本的水平，在那里它们将提供热力学和反应动力学分析的方法以及反应过程可视化的有效演示工具。 这些示范也将用于向地区高中的推广，强调基本的化学概念，同时使年轻学生接触到一个重要的、不断发展的利用计算机技术的研究领域。 最后，这个职业规划要求开发一个网络模块，为计算化学概念提供简单的解释和例子;这个网站将被研究生，本科生和高中生访问。 网络模块将是实现本项目所有教育目标的重要工具，包括研究生、本科生和高中生的相关目标。 因此，这些活动的整体影响将是一个具体的工程问题的实验/理论相结合的方法，金属-SiO2界面的化学和教育工具，将鼓励学生使用这种协同方法在处理工程问题的发展一般。

The combined use of ab initio computational chemistry and experimental spectroscopies in addressing engineering problems is becoming an increasingly widespread approach. This CAREER project will emphasize the combination of theory and experiment both in performing fundamental research and in educating students with diverse levels of experience. The research component focuses on development of a new model system that will enable detailed investigations of the chemistry and physics of metal-insulator interfaces. These interfaces are important for an array of applications, including microelectronics engineering, heterogeneous catalysis, and chemical sensing, but have been difficult to study using experiment or theory because they are typically "buried" under a continuous solid layer. In this project, model interfaces that are accessible to both experimental and theoretical techniques will be formed by adsorption of SiO2-like spherosiloxane clusters onto catalytic metal single crystal surfaces. A battery of experimental techniques will be used to characterize the adsorption and reaction of spherosiloxanes, varying the composition and morphology of the metal substrate along with the size of the spherosiloxane clusters. Results from first-principles computations will be used in interpreting experimental observations, helping to understand the molecular-level structure of the interfaces formed. Once characterized, the model interface will be used to study the mechanism for an important application: the detection of H2 gas using metal-oxide-semiconductor devices. Teams of graduate and undergraduate students who participate in this research will gain broad experience in theoretical principles, advanced spectroscopic techniques, and real-world applications.This synergy of theory, spectroscopic techniques, and application development will be emphasized in instructional activities as well. In these efforts, we will exploit the utility of computational chemistry software for aiding students in visualization of chemical reactions at the molecular scale. A new graduate/advanced undergraduate course will focus on analysis of chemical reaction processes in terms of molecular-scale transformations, with students' use of computational chemistry software representing a key component of the course. Molecular modeling simulations will also be introduced on a more basic level in undergraduate courses, where they will provide both a method for analysis of thermodynamics and reaction kinetics and an effective demonstration tool for visualization of reaction processes. These demonstrations will also be used in outreach to area high schools, emphasizing elementary chemistry concepts while at the same time exposing young students to an important, growing area of research that makes use of computer technology. Finally, this career plan calls for development of a web module that provides simple explanations and examples for computational chemistry concepts; this web site will be accessible to graduate, undergraduate, and high school students. The web module will be an essential tool in achieving all the educational goals of this project, including those relevant for graduate, undergraduate, and high school students. Thus, the overall impact of these activities will be the development of both a combined experimental/theoretical approach to a specific engineering problem-the chemistry of metal-SiO2 interfaces-and educational tools that will encourage students to use this synergistic approach in dealing with engineering problems in general.