Reactive and Non-Reactive Force Field Design Guided by Advances in Energy Decomposition Analysis

以能量分解分析进展为指导的反应性和非反应性力场设计

• 批准号: 1955643
• 负责人: Teresa Head-Gordon
• 金额: $ 69.9万
• 依托单位: University of California-Berkeley
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-04-01 至 2024-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1955643&HistoricalAwards=false
• 关键词: Reactive; Non; Force; Field; Design

Teresa Head-Gordon and Martin Head-Gordon of the University of California, Berkeley, are supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop advanced force-fields. In chemical research, computer-based molecular simulations are an indispensible complement to experimental probes of chemical reactions. Simulation is used to understand the role that solvents (usually liquids that disperse the starting materials and products) play in chemical reactions. Such simulations use force fields to propagate the motions of the molecules. Force fields are empirical functions describe how the potential energy of a system varies with the position of the atoms and molecules both accurately and inexpensively. Molecular simulations advance by improving the accuracy of the force field, and via better statistical sampling. The central goal of this research is to pursue rational, next-generation force field design guided by new advances in energy decomposition analysis (EDA). An EDA takes advanced quantum mechanical calculations on groups of molecules, and distills the interaction energy of the molecules into a sum of terms that captures the repulsive and attractive physical driving forces. These terms provide valuable data to inform the design and parameterization of the new force fields. These developments also yield new computational tools that are useful to other chemists, and are made available to them as software, following validation and pilot applications. The research provides very strong training for graduate students in advanced theory, software development, and chemical applications. A new Berkeley Professional Master's program in Molecular Simulation and Software Engineering (MSSE) is launching in 2020, to train post-baccalaureate students in computational molecular science, best software engineering practices, and the leadership and management skills needed to drive software enterprises. A special topics class on computational quantum chemistry for non-specialists using a freely available e-book, including the EDA methods developed under NSF support is being developed. The Computational Chemistry for Transfer Students (CC-TS) undergraduate research program, targeting junior-level transfer students is also supported. The target of this research is the completion of a protein force field with methodology that generalizes to other complex condensed phase chemistry that involves perturbations to the electron density without changing bonded chemistry. A new EDA capability is being developed for key classes of intramolecular interactions enabling physical insight into conformational equilibria and torsional potentials. The EDA framework is being extended to include polarizable continuum solvent models to enable study of intermolecular interactions, under different dielectric environments. To advance modeling of reactive chemistry in the condensed phase, the improved non-bonded interactions developed for the non-reactive models will be utilized to yield higher accuracy than current models and to allow seamless mixing of reactive and non-reactive force fields. Additionally, the creation of a next generation post-SCF EDA enables analysis of changes in chemical bonding to better characterize the bond order terms (or their equivalent) within the reactive force field. These models and methods are deployed for selected applications, including evaluation of condensed phase terahertz spectroscopic observables, unraveling the driving forces of molecular torsion balance species in solution and in gas phase, and probing the role of electrostatic solvation versus molecular solvation in mediating physical forces.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.

加州大学伯克利分校的Teresa Head-Gordon和Martin Head-Gordon获得了化学系化学理论、模型和计算方法项目的奖励，以开发先进的力场。 在化学研究中，基于计算机的分子模拟是化学反应实验探针不可或缺的补充。 模拟用于了解溶剂（通常是分散起始材料和产品的液体）在化学反应中的作用。这种模拟使用力场来传播分子的运动。力场是一种经验函数，它精确而廉价地描述了一个系统的势能如何随原子和分子的位置而变化。分子模拟通过提高力场的准确性和更好的统计抽样来推进。这项研究的中心目标是追求合理的，下一代力场设计的能量分解分析（EDA）的新进展的指导下。EDA对分子组进行高级量子力学计算，并将分子的相互作用能提取为捕获排斥和吸引物理驱动力的项之和。这些术语为新力场的设计和参数化提供了有价值的数据。这些发展还产生了对其他化学家有用的新的计算工具，并在验证和试点应用后作为软件提供给他们。 该研究为高级理论，软件开发和化学应用方面的研究生提供了非常强的培训。分子模拟和软件工程（MSSE）的一个新的伯克利专业硕士课程将于2020年推出，以培养计算分子科学，最佳软件工程实践以及驱动软件企业所需的领导和管理技能的学士后学生。正在开发一个关于计算量子化学的特别主题课程，供非专业人员使用免费提供的电子书，包括在NSF支持下开发的EDA方法。计算化学转学生（CC-TS）本科研究计划，针对初中转学生也得到了支持。这项研究的目标是完成蛋白质力场的方法，推广到其他复杂的凝聚相化学，涉及电子密度的扰动，而不改变键合化学。一个新的EDA能力正在开发的关键类分子内相互作用，使物理洞察到构象平衡和扭转潜力。EDA框架正在扩展到包括极化连续溶剂模型，使分子间相互作用的研究，在不同的介电环境。为了推进凝聚相中反应性化学的建模，将利用为非反应性模型开发的改进的非键合相互作用来产生比当前模型更高的准确性，并允许反应性和非反应性力场的无缝混合。此外，创建下一代后SCF EDA能够分析化学键的变化，以更好地表征反应力场内的键级项（或其等效项）。这些模型和方法被部署用于选定的应用，包括评估凝聚相太赫兹光谱观测值，解开溶液和气相中分子扭转平衡物质的驱动力，该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准。

项目成果

Effective Two-Body Interactions

• DOI: 10.1021/acs.jpca.1c05677
• 发表时间: 2021-08-30
• 期刊: JOURNAL OF PHYSICAL CHEMISTRY A
• 影响因子: 2.9
• 作者: Mackie, Cameron;Zech, Alexander;Head-Gordon, Martin
• 通讯作者: Head-Gordon, Martin

Revisiting the Bonding Model for Gold(I) Species: The Importance of Pauli Repulsion Revealed in a Gold(I)-Cyclobutadiene Complex.

• DOI: 10.1002/anie.202202019
• 发表时间: 2022-05-23
• 期刊: Angewandte Chemie (International ed. in English)

Software for the frontiers of quantum chemistry: An overview of developments in the Q-Chem 5 package.

• DOI: 10.1063/5.0055522
• 发表时间: 2021-08-28
• 期刊: The Journal of chemical physics

NewtonNet: a Newtonian message passing network for deep learning of interatomic potentials and forces.

• DOI: 10.1039/d2dd00008c
• 发表时间: 2022-06-13
• 期刊: DIGITAL DISCOVERY
• 作者: Haghighatlari, Mojtaba;Li, Jie;Guan, Xingyi;Zhang, Oufan;Das, Akshaya;Stein, Christopher J.;Heidar-Zadeh, Farnaz;Liu, Meili;Head-Gordon, Martin;Bertels, Luke;Hao, Hongxia;Leven, Itai;Head-Gordon, Teresa
• 通讯作者: Head-Gordon, Teresa

Dissociation of HCl in water nanoclusters: an energy decomposition analysis perspective

HCl 在水纳米团簇中的解离：能量分解分析视角

• DOI: 10.1039/d1cp04587c
• 发表时间: 2021
• 期刊: Physical Chemistry Chemical Physics
• 影响因子: 3.3
• 作者: Zech, Alexander;Head-Gordon, Martin
• 通讯作者: Head-Gordon, Martin