Animating Lewis Dots: the development of transferable sub-atomistic force fields for efficient, intuitive, turnkey simulations of chemical reactions

路易斯点动画：开发可转移的亚原子力场，用于高效、直观、统包的化学反应模拟

• 批准号: 1855923
• 负责人: Judith Herzfeld
• 金额: $ 43.5万
• 依托单位: Brandeis University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-06-15 至 2022-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1855923&HistoricalAwards=false
• 关键词: Animating; Lewis; Dots; development; transferable

Judith Herzfeld of Brandeis University is supported by an award from the Chemical Theory, Models and Computational Methods program to develop reactive force fields for molecular simulation. Her goal is to make theory a nimbler partner with experiment in exploring and understanding the pathways of complex chemical reactions. Ideally, computational chemistry should be accurate, versatile, efficient and user-friendly. This is a tall order so computational chemistry usually prioritizes only a couple of these goals. Herzfeld and coworkers are developing a new approach that seeks to combine accurate versatility with efficiency and user-friendliness. This work is expected to provide researchers with useful computational tools for simulating chemical reactions in a broad range of realistic solvents. This research may have impacts in catalysis and advanced manufacturing. The project also provides educators with visualization tools that are useful for instructing students in the mechanisms of chemical reactions. The handiest tool for thinking and communicating about reactions has been the semi-classical "Lewis dot" picture. This century old rubric is "classical" in the sense of thinking of valence electrons and kernels as independently mobile particles, and "semi" in the sense that these particles follow non-classical rules. Herzfeld's work seeks to provide a quantitative version of this heretofore qualitative picture by developing force fields for Lewis' sub-atomistic particles that effectively and efficiently incorporate quantum effects. This project builds on their earlier work on the acid-base chemistry of non-metals (with paired valence electrons) and the ionization and spin states of nonmetals and metals (with valence electrons modeled singly). In particular, the researchers are using an improved understanding of the exchange contributions to the energy to extend the range of applicability. The work involves training, validating and demonstrating the potentials that describe the interactions between the particles. The goal is for these simulations be "turn-key" in the sense of requiring no input as to reaction intermediates or products.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.

布兰迪斯大学的Judith Herzfeld获得了化学理论、模型和计算方法项目的奖励，以开发用于分子模拟的反应力场。她的目标是在探索和理解复杂化学反应的途径时，使理论与实验成为更灵活的伙伴。理想情况下，计算化学应该是准确的、通用的、高效的和用户友好的。这是一个很高的要求，所以计算化学通常只优先考虑其中的几个目标。赫茨菲尔德和他的同事们正在开发一种新的方法，寻求将精确的多功能性与效率和用户友好性结合起来。这项工作有望为研究人员提供有用的计算工具来模拟各种实际溶剂中的化学反应。该研究对催化和先进制造具有一定的指导意义。该项目还为教育工作者提供可视化工具，这些工具对指导学生化学反应的机制很有用。思考和交流反应的最方便的工具是半经典的“刘易斯点”图。这个世纪的古老规则是“经典”的，因为它认为价电子和核是独立移动的粒子，而“半”的意思是这些粒子遵循非经典规则。赫茨菲尔德的工作旨在通过开发刘易斯亚原子粒子的力场，有效地结合量子效应，为迄今为止的定性图景提供一个定量版本。这个项目建立在他们早期对非金属的酸碱化学（用成对的价电子）和非金属和金属的电离和自旋状态（用单独的价电子建模）的研究基础上。特别是，研究人员正在利用对能量交换贡献的更好理解来扩大适用范围。这项工作包括训练、验证和演示描述粒子之间相互作用的势能。我们的目标是让这些模拟在不需要输入反应中间体或产物的意义上成为“交钥匙”。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。