Quantum Dynamics with Nuclear Quantum Effects: a Hhierarchical Methodology for Large Molecular Systems

具有核量子效应的量子动力学：大分子系统的层次方法论

• 批准号: 2308922
• 负责人: Sophya Garashchuk
• 金额: $ 53万
• 依托单位: University of South Carolina at Columbia
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-08-01 至 2026-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2308922&HistoricalAwards=false
• 关键词: Quantum; Dynamics; Nuclear; Effects; Hhierarchical

With support from the Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry, and the Established Program to Stimulate Competitive Research (EPSCoR), Professor Sophya Garashchuk of the University of South Carolina will develop theoretical and computational methods incorporating the quantum behavior of the nuclei within molecules and materials. This research aims to gain in-depth understanding of the properties of molecular assemblies and nanomaterials and their interactions with light, electric current and heat through the first-principles modeling and theoretical analysis, spanning several orders of magnitude in time and space. The developed methodology will be applied to experimental systems, helping to elucidate the intrinsic mechanisms of chemical reactivity and charge and energy transfer, and to predict the rates of such processes. Modeling system properties and responses to external stimuli, such as temperature, electric and magnetic fields, will guide experiment, accelerating the development of new materials and molecular devices for wide-range applications from fuel cells to catalysis, to quantum technologies. Professor Garashchuk's research and educational activities will contribute to the development of the emerging quantum information science and technology work force. She will actively promote computational chemistry tools in education and research among students and scientists at her university and at predominantly undergraduate institutions in the state of South Carolina. Her research group will participate in K-12 science demonstrations and science showcases highlighting the role of chemistry in the forefront scientific advances and in everyday technologies. These activities will broaden participation of the underrepresented groups in research and communicate STEM (science, technology, engineering and mathematics) achievements to the general public of South Carolina, a state geographically underrepresented in the global research enterprise.The theoretical framework being developed under this award will include a quantum mechanical description of light nuclei, such as protons, ubiquitous in aqueous solutions and biological and nanodevice environments. Because of the exponential scaling of the numerical cost, this rigorous treatment is feasible for just a few nuclei, and it will be reserved for the chemically active light nuclei. This level of description will be merged with the classical representations of the larger molecular environment affecting the energy and charge flow due to small amplitude nuclear motion and structural rearrangements. This hierarchical approach will be based on the time-dependent Gaussian bases tailored to an evolving wavefunction for the fully quantum nuclei, integrated with a simplified quantum (e. g. thawed Gaussian) description of the heavy nuclei, compatible with on-the-fly electronic structure evaluation, and will be extended to electronically nonadiabatic processes. Garashchuk will also develop nuclear-subspace factorized electron-nuclear dynamics based on probability density continuity. This formalism will be used to target molecular dynamics involving a large number of electronic states coupled through nuclear motion and external fields, e.g. molecule/nanoparticle systems. In the area of education and broader impacts, Garashchuk will train junior researchers in theoretical, computational chemistry, and high-performance computing; she will facilitate use of computational chemistry tools by experimental colleagues through formal teaching and collaborative projects.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，刺激竞争研究的既定计划（EPSCOR），南卡罗来纳大学的Sophya Garashchuk教授将开发理论和计算方法，将分子和材料中核的量子行为纳入量子。这项研究旨在深入了解分子组件和纳米材料的性质及其与光，电流和热量通过第一原理建模和理论分析的相互作用，涵盖了时间和空间的几个数量级。开发的方法将应用于实验系统，有助于阐明化学反应性，电荷和能量传递的内在机制，并预测此类过程的速率。建模系统的特性和对外部刺激的响应（例如温度，电场和磁场）将指导实验，加速新材料和分子设备的开发，以从燃料电池到催化到量子技术，以进行大型应用。 Garashchuk教授的研究和教育活动将有助于新兴量子信息科学和技术劳动力的发展。她将积极促进大学和科学家在南卡罗来纳州的学生和科学家的教育和研究中的计算化学工具。 她的研究小组将参加K-12科学示范和科学，展示了化学在最前沿的科学进步和日常技术中的作用。 These activities will broaden participation of the underrepresented groups in research and communicate STEM (science, technology, engineering and mathematics) achievements to the general public of South Carolina, a state geographically underrepresented in the global research enterprise.The theoretical framework being developed under this award will include a quantum mechanical description of light nuclei, such as protons, ubiquitous in aqueous solutions and biological and nanodevice环境。由于数值成本的指数缩放率，这种严格的处理仅适用于几个核，并且将保留给化学活动的光核。这种描述级别将与较大的分子环境的经典表示相吻合，这些分子环境会影响幅度较小的核运动和结构重排引起的能量和电荷流。这种分层方法将基于针对完全量子核的不断发展的波函数量身定制的时间依赖性的高斯基地，该核与重型核的简化量子（例如，融化的高斯）描述集成在一起，并将其与实时的电子结构评估兼容，并将扩展到电子上不添加电子粘贴过程。 Garashchuk还将基于概率密度连续性开发核空域分解的电子核动力学。这种形式主义将用于靶向分子动力学，涉及大量通过核运动和外部磁场耦合的电子状态，例如分子/纳米颗粒系统。在教育领域和更广泛的影响方面，Garashchuk将培训初级研究人员的理论，计算化学和高性能计算；她将通过正式的教学和协作项目来促进实验同事使用计算化学工具。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的知识分子优点和更广泛的影响评估标准通过评估来支持的。