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.

在化学系化学理论、模型和计算方法(CTMC)计划和既定的刺激竞争研究计划(EPSCoR)的支持下，南卡罗来纳大学的Sophya Garashchuk教授将开发结合分子和材料中原子核的量子行为的理论和计算方法。本研究旨在通过第一性原理建模和理论分析，跨越几个数量级的时间和空间，深入了解分子组装和纳米材料的性质以及它们与光、电流和热的相互作用。开发的方法将应用于实验系统，帮助阐明化学反应以及电荷和能量转移的内在机制，并预测这些过程的速率。对系统特性和对外界刺激(如温度、电场和磁场)的响应进行建模将指导实验，加速开发新材料和分子器件，用于从燃料电池到催化，再到量子技术的广泛应用。加拉舒克教授的研究和教育活动将有助于新兴的量子信息科学和技术工作队伍的发展。她将在她所在大学和南卡罗来纳州以本科生为主的机构的学生和科学家中积极推动计算化学工具在教育和研究中的应用。她的研究小组将参加K-12科学演示和科学展示，强调化学在前沿科学进步和日常技术中的作用。这些活动将扩大未被充分代表的群体在研究中的参与，并向南卡罗来纳州的公众传播STEM(科学、技术、工程和数学)成果，南卡罗来纳州是一个地理上在全球研究企业中代表性不足的州。根据该奖项开发的理论框架将包括对轻核的量子力学描述，如质子，普遍存在于水溶液以及生物和纳米设备环境中。由于数值成本的指数比例，这种严格的处理方法只适用于少数几个原子核，并将保留用于化学活性较轻的原子核。这一水平的描述将与由于小幅度核运动和结构重排而影响能量和电荷流的更大分子环境的经典表示相结合。这种分层方法将基于为全量子核的演化波函数量身定做的随时间变化的高斯基，与重核的简化量子(例如解冻的高斯)描述相结合，与即时电子结构评估兼容，并将扩展到电子非绝热过程。Garashchuk还将在概率密度连续性的基础上发展核子空间分解的电子-核动力学。这种形式将被用来针对分子动力学，包括通过核运动和外场耦合的大量电子态，例如分子/纳米粒子系统。在教育和更广泛的影响领域，Garashchuk将在理论、计算化学和高性能计算方面培训初级研究人员；她将通过正式的教学和合作项目促进实验同事使用计算化学工具。该奖项反映了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。