Molecular Electronic Structure Theory: Methods and Applications

分子电子结构理论：方法与应用

• 批准号: 1661604
• 负责人: Henry Schaefer III
• 金额: $ 45万
• 依托单位: University of Georgia Research Foundation Inc
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-08-01 至 2022-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1661604&HistoricalAwards=false
• 关键词: Molecular; Electronic; Structure; Theory; Methods; Molecular; Electronic; Structure; Theory; Methods

Henry (Fritz) Schaeffer is supported by an award from the Chemical Theory, Models and Computational Method program in the Division of Chemistry to develop new computational and theoretical approaches for quantum chemistry. This project contributes to the understanding of atoms, molecules, and molecular assemblies in the gas, liquid, and solid phases. These are the elementary components of the chemistry that underlies our understanding of materials from lasers to superconductors and on to biochemical systems. The most important equation in science, the Schrodinger Equation, is the key to new discoveries in science and engineering, areas dedicated to advances of importance to humankind. While one speaks of the Schrodinger Equation, in fact there is a different Schrodinger Equation for every different molecular system. These equations are extremely complicated for systems of broad, general interest. The practical solutions of the Schrodinger Equation require a profound mastery of both mathematics and physics to allow the derivation of important new methods. Dr. Schaefer and his research team excel in the development and application of mathematical physics, algorithm design, and computer science to achieve these goals. An important new method being developed is density cumulant functional theory. The research group also applies these new methods to the solution of important problems in the chemical sciences. Their research on manganese CO2 reduction, palladium catalysts, silicon chemistry, gallium nitride nanotubes, the CF3 substitutes SF5 and PF4, iodine clusters, and atmospheric chemistry, bears upon several areas of technological concern. This project focuses on the development of new theoretical and computational methods for the understanding and prediction of chemical phenomena. More specifically, the Schaefer group uses electronic structure theory (quantum chemistry) to innovate, implement, and apply new methods for the description of electron correlation in molecules, one of the most challenging areas of chemical theory. A emphasis of this proposal is the development of multi-reference density cumulant theory (MRDCT). The establishment of MRDCT involves the outline of the new formalism, design of effective algorithms, careful coding of the method, and assessment through benchmarks. Applications of new and existing theoretical methods include molecular architectures; spectroscopy (microwave, infrared, electronic, Raman); potential energy surfaces; energetics; reactions via organometallic catalysts (often involving the earth abundant metal manganese); palladium catalysis for C-H bond activation and reductive elimination; examination of the biologically important class of reactions between persulfides (R1SSR2) and sulfides (R2SR4); and collaborations with experiment toward the synthesis of critically important new main group chemistry targets. Broader impacts of the research include the education of a significant number of gifted Ph.D. students (16 in the group currently). Professor Schaefer aggressively and successfully recruits women and underrepresented minorities for their Ph.D. studies. These doctoral students (110 graduated to date, including 23 women) almost uniformly go on to highly fruitful scientific careers in academia, government laboratories, and industry. Schaefer's research group reaches out to local students in elementary, middle, and high schools. The Schaefer group is active in the development PSI4, a freely-available, open source, comprehensive, and widely used suite of quantum chemistry computer programs. It is especially easy for scientists to add new features to the PSI4 code.

亨利（Fritz）Schaeffer得到了化学理论，模型和计算方法计划的奖励，以开发量子化学的新计算和理论方法。该项目有助于理解气体，液体和固体相的原子，分子和分子组件。这些是化学的基本组成部分，是我们对从激光到超导体以及生化系统的材料的理解的基础。科学中最重要的方程式，即施罗宾格方程，是科学和工程学新发现的关键，该领域致力于对人类的重要性发展。虽然有人谈到了施罗丁格方程，但实际上每个不同的分子系统都有不同的schrodinger方程。对于广泛而普遍的兴趣系统，这些方程非常复杂。 Schrodinger方程的实际解决方案需要对数学和物理学的深刻掌握，以允许推导重要的新方法。 Schaefer博士和他的研究团队在数学物理，算法设计和计算机科学的开发和应用方面表现出色，以实现这些目标。正在开发的重要新方法是密度累积功能理论。研究小组还将这些新方法应用于化学科学中重要问题的解决方案。他们对锰二氧化碳减少，钯催化剂，硅化学，氮化盐纳米管，CF3替代品SF5和PF4，碘簇和大气化学的研究都在技术关注的几个领域都承受。 该项目重点是开发新的理论和计算方法，以理解和预测化学现象。更具体地说，Schaefer组使用电子结构理论（量子化学）来创新，实施和应用新方法来描述分子中电子相关性，这是化学理论最具挑战性的领域之一。该提议的重点是多参考密度累积理论（MRDCT）的发展。 MRDCT的建立涉及新形式主义的轮廓，有效算法的设计，仔细编码方法以及通过基准评估。新的和现有理论方法的应用包括分子体系结构；光谱法（微波炉，红外，电子，拉曼）；势能表面；能量学；通过有机金属催化剂的反应（通常涉及地球丰富的金属锰）；用于C-H键激活和还原性消除的钯催化；检查过硫化物（R1SSR2）和硫化物（R2SR4）之间的生物学上重要的反应类别；并与实验合成至关重要的新主要团体化学目标的合作。 该研究的更广泛影响包括对大量有天赋的博士学位进行教育。学生（目前在小组中有16个）。 Schaefer教授积极并成功地招募了妇女，并为其博士学位招募了少数民族。研究。这些博士生（迄今为止有110名毕业，包括23名女性）几乎统一地从事学术界，政府实验室和行业的富有成果的科学职业。 Schaefer的研究小组与小学，中学和高中的当地学生联系。 Schaefer小组活跃于开发PSI4，这是一个自由使用的，开源的，全面的，广泛使用的量子化学计算机程序。科学家特别容易地为PSI4代码添加新功能。