Data-Driven Many-Body Models for Molecular Simulations of Ions in Water: From Ionic Clusters to Concentrated Electrolyte Solutions

用于水中离子分子模拟的数据驱动多体模型：从离子簇到浓缩电解质溶液

• 批准号: 1954895
• 负责人: Francesco Paesani
• 金额: $ 49.06万
• 依托单位: University of California-San Diego
• 依托单位国家: 美国
• 项目类别: Standard 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=1954895&HistoricalAwards=false
• 关键词: Data; Driven; Many; Body; Models

Dr. Francesco Paesani of the University of California-San Diego is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry. A quantitative, molecular-level characterization of the structural, thermodynamic, dynamical, and spectroscopic properties of ions in aqueous environments under different conditions is key to understanding several fundamental processes, including ion-molecule reactions and ion-induced nucleation in the atmosphere, acid-base reactions in solution, ion transport in biological channels, and multiphase processes at air/liquid and solid/liquid interfaces. A unified picture of the behavior of hydrated ions across different phases and in different environments is particularly challenging, requiring a quantitative assessment of competing enthalpic and entropic effects associated with the interplay between ion–ion, ion–water, and water–water interactions, which are further modulated by nuclear quantum effects. By combining data-driven many-body potential energy functions derived entirely from high-level ab initio reference data with both classical and quantum molecular dynamics, Paesani will extend his many-body molecular dynamics (MB-MD) methodology to the modeling of ions in water, from gas-phase clusters to bulk solutions. The MB-MD methodology provides an accurate, yet efficient, theoretical/computational framework for molecular simulations of aqueous systems with high accuracy and predictive power. In this research project Paesani aims to develop a microscopic understanding of single-ion hydration structure and thermodynamics from small gas-phase clusters to bulk solutions in terms of individual many-body contributions, determine single-ion hydration free energies and ion–ion association free energies and decompose them in terms of elementary ion–water and water–water many-body effects, and characterize water hydrogen-bond structure and dynamics in electrolyte solutions as a function of ion concentration and composition, disentangling ion–ion, ion–water and water–water contributions. The theoretical/ computational methodology developed as part of the proposed research will have broad impact on a wide range of user communities from chemistry to materials science and biology, and will involve the training and education of high school, undergraduate and graduate students who will acquire a solid foundation in theoretical, computational, and physical chemistry. The interdisciplinary nature of the proposed project will provide the students with the opportunity to work at the interface of different disciplines which will prepare them for a wide range of careers.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.

加州大学圣地亚哥分校的 Francesco Paesani 博士获得了化学系化学理论、模型和计算方法项目的资助，该项目对结构、热力学、动力学和光谱进行定量、分子水平表征。不同条件下水环境中离子的性质是理解几个基本过程的关键，包括大气中的离子分子反应和离子诱导成核、溶液中的酸碱反应、生物通道中的离子传输、空气/液体和固体/液体界面的多相过程尤其具有挑战性，需要对与离子之间相互作用相关的竞争性焓和熵效应进行定量评估。离子、离子-水和水-水相互作用，通过将完全源自高级从头计算参考数据的数据驱动的多体势能函数与经典和量子分子相结合，进一步受到核量子效应的调节。动力学方面，Paesani 将把他的多体分子动力学 (MB-MD) 方法扩展到水中离子的建模，从气相簇到本体溶液，MB-MD 方法提供了一个准确而高效的理论/计算框架。在这个研究项目中，Paesani 旨在对单离子水合结构和从小型气相簇到整体解决方案的热力学进行微观理解，以实现对单个多体的贡献。确定单离子水合自由能和离子-离子缔合自由能，并将它们分解为基本离子-水和水-水多体效应，并将电解质溶液中的水氢键结构和动力学表征为离子的函数作为拟议研究的一部分而开发的理论/计算方法将对从化学到材料科学和生物学的广泛用户群体产生广泛影响。将涉及到对高中生、本科生和研究生的培训和教育，使他们在理论、计算和物理化学方面打下坚实的基础。拟议项目的跨学科性质将为学生提供在不同学科交叉领域工作的机会。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Data-driven many-body potentials from density functional theory for aqueous phase chemistry

水相化学密度泛函理论的数据驱动多体势

• DOI: 10.1063/5.0129613
• 发表时间: 2023-03
• 期刊: Chemical Physics Reviews
• 作者: Palos, Etienne;Dasgupta, Saswata;Lambros, Eleftherios;Paesani, Francesco
• 通讯作者: Paesani, Francesco

Accurate Modeling of Bromide and Iodide Hydration with Data-Driven Many-Body Potentials

利用数据驱动的多体势对溴化物和碘化物水合进行精确建模

• DOI: 10.1021/acs.jpcb.2c04698
• 发表时间: 2022-10
• 期刊: The Journal of Physical Chemistry B
• 作者: Caruso, Alessandro;Zhu, Xuanyu;Fulton, John L.;Paesani, Francesco
• 通讯作者: Paesani, Francesco

Hydration Structure of Na + and K + Ions in Solution Predicted by Data-Driven Many-Body Potentials

数据驱动的多体势预测溶液中 Na 和 K 离子的水合结构

• DOI: 10.1021/acs.jpcb.2c05674
• 发表时间: 2022-11
• 期刊: The Journal of Physical Chemistry B
• 作者: Zhuang, Debbie;Riera, Marc;Zhou, Ruihan;Deary, Alexander;Paesani, Francesco
• 通讯作者: Paesani, Francesco

Data-driven many-body models enable a quantitative description of chloride hydration from clusters to bulk

数据驱动的多体模型能够定量描述从簇到块状的氯化物水合

• DOI: 10.1063/5.0059445
• 发表时间: 2021-08
• 期刊: The Journal of Chemical Physics
• 作者: Caruso, Alessandro;Paesani, Francesco
• 通讯作者: Paesani, Francesco