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Molecular Electronic Structure Theory: Methods and Applications

分子电子结构理论：方法与应用

基本信息

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

项目摘要

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.

Henry(Fritz)Schaeffer得到了化学部化学理论、模型和计算方法计划的支持，为量子化学开发新的计算和理论方法。该项目有助于理解气相、液态和固相中的原子、分子和分子组装。这些是化学的基本组成部分，它奠定了我们对材料的理解，从激光到超导体，再到生化系统。科学中最重要的方程，薛定谔方程，是科学和工程领域新发现的关键，这些领域致力于对人类具有重要意义的进步。虽然人们谈论薛定谔方程，但实际上每个不同的分子体系都有不同的薛定谔方程。这些方程对于广泛而普遍感兴趣的系统来说是极其复杂的。薛定谔方程的实际解需要对数学和物理都有深刻的掌握，才能推导出重要的新方法。Schaefer博士和他的研究团队擅长数学物理、算法设计和计算机科学的开发和应用，以实现这些目标。一种重要的新方法是密度累积量泛函理论。研究小组还将这些新方法应用于解决化学科学中的重要问题。他们在二氧化碳锰还原、钯催化剂、硅化学、氮化镓纳米管、取代SF5和PF4的CF3、碘团簇和大气化学等方面的研究涉及几个技术关注的领域。这个项目的重点是开发新的理论和计算方法来理解和预测化学现象。更具体地说，Schaefer小组使用电子结构理论(量子化学)来创新、实施和应用描述分子中电子相关性的新方法，这是化学理论中最具挑战性的领域之一。这一建议的重点是发展多参考密度累积量理论(MRDCT)。MRDCT的建立涉及到新形式主义的概述、有效算法的设计、方法的仔细编码以及通过基准进行评估。新的和现有的理论方法的应用包括：分子结构；光谱学(微波、红外、电子、拉曼)；势能面；能量学；通过有机金属催化剂的反应(通常涉及地球上丰富的金属锰)；钯催化C-H键的活化和还原消除；过硫化物(R1SSR2)和硫化物(R2SR4)之间具有生物重要性的一类反应的检验；以及与实验合作合成关键的新的主族化学目标。这项研究的更广泛影响包括对相当数量的有天赋的博士生(目前该群体中有16人)的教育。Schaefer教授积极而成功地招募女性和少数族裔代表不足的人攻读博士学位。这些博士生(到目前为止有110名毕业生，其中包括23名女性)几乎一致地在学术界、政府实验室和工业界从事卓有成效的科学事业。Schaefer的研究小组接触到了当地小学、初中和高中的学生。Schaefer团队积极参与PSI4的开发，PSI4是一套免费、开源、全面且广泛使用的量子化学计算机程序。对于科学家来说，为PSI4代码添加新功能尤其容易。

项目成果

期刊论文数量（51）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Formation of Formic Acid Derivatives through Activation and Hydroboration of CO 2 by Low-Valent Group 14 (Si, Ge, Sn, Pb) Catalysts

低价14族（Si、Ge、Sn、Pb）催化剂活化和硼氢化CO 2 形成甲酸衍生物

DOI：
10.1021/acs.jpca.9b11648
发表时间：
2020
期刊：
The Journal of Physical Chemistry A
影响因子：
0
作者：
Villegas-Escobar, Nery;Schaefer, Henry F.;Toro-Labbé, Alejandro
通讯作者：
Toro-Labbé, Alejandro

PES-Learn: An Open-Source Software Package for the Automated Generation of Machine Learning Models of Molecular Potential Energy Surfaces

DOI：
10.1021/acs.jctc.9b00312
发表时间：
2019-08-01
期刊：
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
影响因子：
5.5
作者：
Abbott, Adam S.;Turney, Justin M.;Schaefer, Henry F., III
通讯作者：
Schaefer, Henry F., III

Using an iterative eigensolver and intertwined rank reduction to compute vibrational spectra of molecules with more than a dozen atoms: Uracil and naphthalene

使用迭代本征解算器和交织的等级约简来计算具有十多个原子的分子的振动光谱：尿嘧啶和萘

DOI：
10.1063/1.5039147
发表时间：
2018
期刊：
The Journal of Chemical Physics
影响因子：
0
作者：
Thomas, Phillip S.;Carrington, Tucker;Agarwal, Jay;Schaefer, Henry F.
通讯作者：
Schaefer, Henry F.

π-Hydrogen Bonding Probes the Reactivity of Aromatic Compounds: Nitration of Substituted Benzenes

DOI：
10.1021/acs.jpca.8b12508
发表时间：
2019-02-07
期刊：
JOURNAL OF PHYSICAL CHEMISTRY A
影响因子：
2.9
作者：
Galabov, Boris;Koleva, Gergana;Schaefer, Henry F.
通讯作者：
Schaefer, Henry F.

Alternative modes of bonding of C 4 F 8 units in mononuclear and binuclear iron carbonyl complexes

单核和双核羰基铁络合物中 C 4 F 8 单元的替代键合模式

DOI：
10.1039/c9nj00882a
发表时间：
2019
期刊：
New Journal of Chemistry
影响因子：
3.3
作者：
Huang, Liping;Li, Jing;Li, Guoliang;Xie, Yaoming;King, R. Bruce;Schaefer, Henry F.
通讯作者：
Schaefer, Henry F.