Minimally Empirical, First Principles-Derived Reactive Potential for Accelerated Simulations of Chemically Interacting Systems

用于加速模拟化学相互作用系统的最小经验、第一原理推导的反应势

• 批准号: 2154781
• 负责人: Alexander Mironenko
• 金额: $ 38.03万
• 依托单位: University of Illinois at Urbana-Champaign
• 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: 2022-06-15 至 2025-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2154781&HistoricalAwards=false
• 关键词: Minimally; Empirical; First; Principles; Derived

With support from the Chemical Theory, Models, and Computational Methods (CTMC) program in the Division of Chemistry, Alex Mironenko of the University of Illinois at Urbana-Champaign is developing minimally empirical reactive interatomic potentials from first principles for accelerating chemical reaction simulations and materials discoveries. Quantum chemical methods being developed over the last 100 years have led to new molecules, materials, and reactions predicted on a computer, reducing the amount of costly trial-and-error experimentation. The methods, however, remain too expensive to describe all intricacies of chemical transformations. Data-driven approximate methods – so-called interatomic potentials – are more affordable but often miss essential physics and require large, expensive data sets for their accuracy. Mironenko will develop interatomic potentials that will incorporate all required physics at a low cost using an overlooked “chemical pseudo-potential” theory introduced in the 1960s. His research group will implement the method using general-purpose software and assess its performance on a chemical reaction of significance to renewable energy. More broadly, the technique aims to quantify and unify fundamental concepts of chemical reactivity and will be integrated into educational modules for both undergraduate and graduate students. This project will generalize the minimally empirical reactive potential, demonstrated for the simplest hydrogen clusters, to main-group elements containing s and p valence orbitals. Several hypotheses and ideas pertaining to the method will be tested, including, but not limited to (1) electronegativity equilibration, (2) effective atomic pseudo-potentials, and (3) analytical bond orders derived from the underlying quantum theory. The method will be implemented using general-purpose, parallelizable open-access software, designed to compute the reactive potential energy surface at a low computational cost. The method will be used to study the mechanism of organocatalytic C-C coupling of formaldehyde to form platform chemicals - C3 oxygenates. The choice is motivated by its impact and relative simplicity, enabling direct comparison of predictions with state-of-the-art ab initio methods. If successful, the proposed method will pave the way to systematically derived, minimally empirical, and transferable reactive potentials, thereby accelerating data generation and further enabling predictive computational chemistry, catalysis, and materials science. The research also has the potential to create new knowledge about the fundamental origins of elementary, textbook electronic structure theories (Huckel, molecular orbital theory), potentially opening up new approaches to the description/teaching of theoretical physical chemistry, in general.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.

在化学系化学理论、模型和计算方法(CTMC)计划的支持下，伊利诺伊大学厄巴纳-香槟分校的Alex Mironenko正在根据第一原理开发最小经验的反应原子间势，以加速化学反应模拟和材料发现。在过去的100年里发展起来的量子化学方法已经导致了在计算机上预测的新分子、材料和反应，减少了昂贵的反复试验的数量。然而，这些方法仍然过于昂贵，无法描述所有错综复杂的化学变化。数据驱动的近似方法--所谓的原子间相互作用势--更实惠，但往往错过了基本的物理学，需要大量昂贵的数据集才能保证准确性。Mironenko将利用20世纪60年代引入的被忽视的“化学赝势”理论来开发原子间势，该势将以低成本结合所有所需的物理。他的研究小组将使用通用软件实现该方法，并评估其在对可再生能源具有重要意义的化学反应中的表现。更广泛地说，这项技术旨在量化和统一化学反应的基本概念，并将被整合到本科生和研究生的教学模块中。这个项目将把最简单的氢团簇的最小经验反应势推广到包含S和p价轨道的主族元素。与该方法有关的几个假设和想法将被检验，包括但不限于(1)电负性平衡，(2)有效原子赝势，和(3)源自基本量子理论的解析键级。该方法将使用通用、可并行的开放访问软件来实现，该软件旨在以较低的计算成本计算无功势能面。该方法将用于研究甲醛有机催化C-C偶联生成平台化合物--C3含氧物的机理。这一选择的动机是其影响力和相对简单性，使预测能够与最先进的从头计算方法进行直接比较。如果成功，所提出的方法将为系统地获得、最小经验和可转移的反应势铺平道路，从而加快数据生成，并进一步使预测计算化学、催化和材料科学成为可能。这项研究还有可能创造关于基本的、教科书中的电子结构理论(休克尔，分子轨道理论)的基本起源的新知识，潜在地为理论物理化学的描述/教学开辟新的途径。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。