Theoretical Studies of Intermolecular Forces

分子间力的理论研究

基本信息

批准号：
2154908
负责人：
Krzysztof Szalewicz
金额：
$ 15万
依托单位：
University of Delaware
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2022
资助国家：
美国
起止时间：
2022-08-01 至 2023-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2154908&HistoricalAwards=false
关键词：
Theoretical Studies Intermolecular Forces

项目摘要

With support from Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry, Professor Krzysztof Szalewicz of University of Delaware is performing quantum-mechanical investigations of clusters of molecules, molecular condensed phases, and biomolecular systems. The properties of such systems are governed by intermolecular (van der Waals) forces: depending on the distance between two molecules, they will either attract or repel each other, a physical law that Richard Feynman considered to be the biggest finding of humanity. Szalewicz and coworkers have developed methods for computing intermolecular forces that are not only among the most accurate and computationally efficient ones, but also provide researchers with a unique ability to interpret properties dependent on intermolecular forces in terms of the four fundamental physical mechanisms: the electrostatic, exchange-repulsion, polarization, and dispersion interactions. Since direct quantum-mechanical calculations are limited to molecular assemblies with a hundred or so atoms, Szalewicz’s group will develop machine-learning methods of extrapolating quantum results to arbitrary-size systems. The importance of this work stems from its ability to predict properties of matter from first principles, i.e., deriving them from equations of quantum mechanics, for arbitrary molecular materials. One example are reliable predictions of crystal structures. Computational design of crystals is of significant importance for pharmaceutical, agrochemical, semiconductor, and energetic materials industries. The fundamental research on intermolecular forces being conducted here has the potential for broad scientific impact across a wide array of fields from materials science to biomolecular, and atmospheric science, to molecular spectroscopy and astrophysics. Broader impacts of this activity include training of graduate students and postdoctoral associates with diverse backgrounds, extensive collaborations with other research groups, organization of conferences and workshops that will disseminate knowledge, participation in award committees and in activities of an international academia, and developments of free software to be used by other researchers.Under this ward, the Szalewicz group is developing and utilizing symmetry-adapted perturbation theory (SAPT) based on monomers described by density-functional theory (DFT), an approach denoted as SAPT(DFT). Machine-learning methods for the generation of force fields derived from SAPT(DFT) calculations will be extended to enable treatment of molecules with soft internal degrees of freedom. These force fields will be used for several systems of current experimental, observational, or technological interest, in particular for predictions of crystal structures from first principles, including difficult cases with polymorphism related to varying conformations of monomers. Other developments of theory will include work on nonlocal-correlation DFT methods that can reliably predict dispersion energies, improved DFT methods that can be paired with accurate dispersion energies, extensions of machine-learning force-field generation methods to three-body nonadditive interactions, and universal force fields based on ab initio computed monomer properties, a step in the direction of physics-based biomolecular force fields. These studies are expected to advance knowledge of the field of intermolecular interactions and to have promise for transformative changes in electronic structure methods, in force-field development techniques, and in crystal structure predictions.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

在化学理论的支持下，在化学划分中的模型和计算方法（CTMC）计划，特拉华大学的Krzysztof Szalewicz教授正在对分子，分子凝结相和生物分子系统的簇，分子凝结相的簇进行量子力学研究。此类系统的性质受分子间（范德华）力控制：根据两个分子之间的距离，它们将互相吸引或驱逐，这是理查德·费曼（Richard Feynman）认为是人类最大发现的物理定律。 Szalewicz及其同事开发了计算分子间力的方法，这些力不仅是最准确和计算上有效的力之一，而且还为研究人员提供了独特的能力，可以根据四种基本物理机制来解释依赖分子间力的特性：静电，交换，交换，换层，偏振，偏振和分散互动。由于直接的量子力学计算仅限于具有一百个原子的分子组件，因此Szalewicz的组将开发出将量子结果推送到任意大小的系统的机器学习方法。 The importance of this work plants from its ability to predict properties of matter from first principles, i.e., deriving them from equations of quantum mechanics, for arbitrary molecular materials.一个例子是对晶体结构的可靠预测。晶体的计算设计对于药物，农业化学，半导体和能量材料行业至关重要。此处进行的关于分子间力的基本研究具有从材料科学到生物分子和大气科学到分子光谱和天体物理学的广泛领域的广泛科学影响。这项活动的更广泛的影响包括对研究生的培训和具有潜水背景的博士后同事，与其他研究小组的广泛合作，会议和研讨会的组织，这些组织将分散知识，参与奖励承诺以及国际学术界的活动，以及其他研究人员使用的自由软件的发展。关于密度功能理论（DFT）描述的单体，一种表示为SAPT（DFT）的方法。将扩展从SAPT（DFT）计算得出的力场生成的机器学习方法，以实现具有软内部自由度的分子处理。这些力场将用于当前实验，观察性或技术兴趣的多种系统，尤其是针对第一原理的晶体结构的预测，包括与单体不同会议有关的困难病例。 Other developments of theory will include work on nonlocal-correlation DFT methods that can reliably predict dispersion energies, improved DFT methods that can be paired with accurate dispersion energies, extensions of machine-learning force-field generation methods to three-body nonadditive interactions, and universal force fields based on ab initio computed monomer properties, a step in the direction of physics-based biomolecular force fields.这些研究有望提高对分子间相互作用领域的了解，并有望在电子结构方法，力场发展技术和晶体结构预测中对变革性变化。该奖项反映了NSF的法定任务，并被认为是通过基金会的知识绩效和更广泛的影响审查的审查标准来通过评估来通过评估来支持的。