Multi-Configuration Pair-Density Functional Theory

多配置对密度泛函理论

• 批准号: 1464536
• 负责人: Laura Gagliardi
• 金额: $ 55.5万
• 依托单位: University of Minnesota-Twin Cities
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2015
• 资助国家: 美国
• 起止时间: 2015-07-01 至 2018-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1464536&HistoricalAwards=false
• 关键词: Multi; Configuration; Pair; Density; Functional

With this award, the Chemical Theory, Models and Computational Methods Program in the Chemistry Division is supporting Professors Laura Gagliardi and Donald G. Truhlar of the University of Minnesota to develop theoretical methods and tools to describe the electronic structure of very important classes of molecules that are difficult to study by most widely used, established approaches. In particular, density functional theory (DFT) methods have become the "workhorse" of modern quantum mechanical methods for large and complex molecular systems. The planned research combines the particular expertise of the Gagliardi and Truhlar research gruops to develop a method that draws on aspects of each of their individual research. The techniques developed as part of this research will be applicable to molecular systems that are expected to have broad impacts in, among others, the following application areas: chemical dynamics, thermochemistry, environmental chemistry, including atmospheric chemistry and aqueous environments, electrochemistry, catalysis, materials, supramolecular chemistry, biochemistry, and nanotechnology. Thus the work is poised to have long-term implications for health, materials, environmental, and industrial applications. Undergraduates, graduate students and postdoctoral fellows will be trained in modern computational chemistry methods as an integral part of this research. Software developed in the project is distributed free to the community in portable well-documented code.Under this award, the Gagliardi and Truhlar research groups are developing and implementing a new quantum chemical theory, called multiconfiguration pair-density functional theory (MC-PDFT). The project will explore new ways to combine density functional theory with multiconfiguration wave functions for multireference systems. MC-PDFT maintains the correct spin and spatial symmetry of the systems under consideration and, at the same time, avoids any possibility of double counting the electron correlation energy. The scaling of the computational costs of MC-PDFT is seen to hold promise. The method is employed for the determination of chemical properties such as bond energies and electronic excitation energies and for the generation of potential energy surfaces to be used in photochemical applications.

凭借该奖项，化学部的化学理论、模型和计算方法项目正在支持明尼苏达大学的 Laura Gagliardi 和 Donald G. Truhlar 教授开发理论方法和工具来描述非常重要的分子类别的电子结构，而这些分子很难通过最广泛使用的既定方法进行研究。 特别是，密度泛函理论（DFT）方法已成为大型复杂分子系统现代量子力学方法的“主力”。 计划中的研究结合了 Gagliardi 和 Truhlar 研究小组的特殊专业知识，开发出一种利用他们各自研究的各个方面的方法。作为这项研究的一部分开发的技术将适用于预计将在以下应用领域产生广泛影响的分子系统：化学动力学、热化学、环境化学，包括大气化学和水环境、电化学、催化、材料、超分子化学、生物化学和纳米技术。 因此，这项工作将对健康、材料、环境和工业应用产生长期影响。 作为这项研究的一个组成部分，本科生、研究生和博士后将接受现代计算化学方法的培训。 该项目开发的软件以可移植、记录良好的代码形式免费分发给社区。根据该奖项，Gagliardi 和 Truhlar 研究小组正在开发和实施一种新的量子化学理论，称为多配置对密度泛函理论 (MC-PDFT)。该项目将探索将密度泛函理论与多参考系统的多配置波函数相结合的新方法。 MC-PDFT 保持了所考虑系统的正确自旋和空间对称性，同时避免了重复计算电子相关能的任何可能性。 MC-PDFT 计算成本的扩展被认为是有希望的。该方法用于测定化学性质，例如键能和电子激发能，以及生成用于光化学应用的势能表面。