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.

在化学理论，模型和计算方法（CTMC）方案的支持下，乌尔巴纳 - 奇普布（Urbana-Champaign）伊利诺伊大学的Alex Mironenko正在开发最低经验的反应性反应性跨性别潜力，从第一原理加速了化学反应反应模拟和材料发现。在过去的100年中开发的量子化学方法导致了计算机上预测的新分子，材料和反应，从而减少了昂贵的试验和错误实验量。但是，这些方法仍然太昂贵，无法描述化学转化的所有复杂性。数据驱动的近似方法（所谓的原子间电位）更实惠，但通常会错过基本物理学，并且需要大量，昂贵的数据集以便其准确性。 Mironenko将开发原子质潜力，该电位将使用1960年代引入的被忽视的“化学伪电势”理论以低成本结合所有必需的物理学。他的研究小组将使用通用软件实施该方法，并评估其对可再生能源意义的化学反应的性能。从更广泛的角度来看，该技术旨在量化和统一化学反应性的基本概念，并将纳入本科生和研究生的教育模块中。该项目将概括为最简单的氢簇证明的最小经验反应电位，即包含S和P价轨道的主元素。将测试与该方法有关的几种假设和思想，包括但不限于（1）电负性平衡，（2）有效的原子伪电势和（3）源自基本量子理论的分析键顺序。该方法将使用通用的，可行的开放式软件实施，旨在以低计算成本计算反应势能表面。该方法将用于研究甲醛形成平台化学物质的有机催化C -C偶联的机理-C3氧化剂。选择是由于其影响和相对简单性的动机，从而可以直接比较预测与最新的从头算法进行比较。如果成功的话，提出的方法将为系统地得出，最小经验和转移的反应性电位铺平道路，从而加速数据生成并进一步实现预测性计算化学，催化和材料科学。这项研究还具有有关基本，教科书电子结构理论（Huckel，分子轨道理论）的基本起源的新知识的潜力，它可能为理论物理化学的描述/教学开辟了新的方法，一般而言，该奖项反映了NSF的法定任务，并通过评估了基金会的范围和广泛的影响，并通过评估了支持。