Theoretical Studies of Surface Reaction Dynamics

表面反应动力学的理论研究

• 批准号: 2306975
• 负责人: Hua Guo
• 金额: $ 50万
• 依托单位: University of New Mexico
• 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: 2023-07-01 至 2027-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2306975&HistoricalAwards=false
• 关键词: Theoretical; Studies; Surface; Reaction; Dynamics

With support from the Chemical Structure, Dynamics, and Mechanisms-A (CSDM-A) and the Chemical Theory, Models, and Computational Methods (CTMC) Programs in the Division of Chemistry, Professor Hua Guo of the University of New Mexico and his research team aim to advance the fundamental understanding of dynamics for atomic and molecular interactions with metal and semiconductor surfaces using computational methods. Professor Guo and his research group will focus on the computational characterization of elementary processes such as adsorption, desorption, scattering, diffusion, and reaction to provide systematic and comprehensive insights into surface reaction dynamics. The knowledge gained from these fundamental studies has the potential to help establish key principles and predictive models for interfacial phenomena thus allowing for better elucidation of important chemical and physical processes at surfaces ranging from corrosion, device fabrication, and heterogeneous catalysis. The students engaged in this work will gain valuable experience in computational research, which will be enhanced through collaborations with experimentalists. An accurate description of energy dissipation in surface processes via both adiabatic and nonadiabatic pathways is sought using density functional theory (DFT), machine learning, as well as classical, semi-classical, and quantum mechanical methods. DFT will be used for understanding the electronic structure of interfacial systems; machine learning will be used for representing high-dimensional potential energy surfaces and other properties, while a combination of classical, semi-classical, and quantum mechanical methods will also be used for simulating nuclear dynamics. Because adiabatic and nonadiabatic pathways are altered by phonons and electron-hole pairs at surfaces, Professor Guo and his group will investigate how energy flow and bond forming/breaking events vary at metal and semiconductor interfaces. This includes investigations of energy dissipation of hot adsorbates, atomic scattering from semiconductor surfaces, vibrational excitation effects in Eley-Rideal reactions on metals, post-transition state dynamics in decomposition/desorption reactions from metal surfaces, and quantum effects in surface reaction rates on metals. Specific objectives include a better understanding of non-Born-Oppenheimer effects, nuclear quantum effects, and mode specificity in reactivity and energy disposal. Collaboration with experimentalists groups will help guide the computational studies so that the complex interplay of energy transfer and chemical transformation on solid surfaces can be better understood.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.

在化学系化学结构、动力学和机理A(CSDM-A)和化学理论、模型和计算方法(CTMC)计划的支持下，新墨西哥大学的郭华教授和他的研究团队旨在通过计算方法促进对原子和分子与金属和半导体表面相互作用的动力学的基本理解。郭教授和他的研究小组将专注于基本过程的计算表征，如吸附、解吸、散射、扩散和反应，以系统和全面地了解表面反应动力学。从这些基础研究中获得的知识有可能帮助建立界面现象的关键原理和预测模型，从而允许更好地阐明从腐蚀、器件制造到多相催化等表面的重要化学和物理过程。从事这项工作的学生将获得宝贵的计算研究经验，这些经验将通过与实验者的合作得到加强。利用密度泛函理论(DFT)、机器学习以及经典、半经典和量子力学的方法，寻求通过绝热和非绝热路径来准确描述表面过程中的能量耗散。DFT将用于理解界面系统的电子结构；机器学习将用于表示高维势能面和其他性质，而经典、半经典和量子力学方法的组合也将用于模拟核动力学。由于绝热和非绝热路径是由表面的声子和电子-空穴对改变的，郭教授和他的团队将研究金属和半导体界面上的能量流动和键形成/断裂事件的变化。这包括热吸附的能量耗散，半导体表面的原子散射，金属Eley-R反应中的振动激发效应，金属表面分解/脱附反应的后过渡态动力学，以及金属表面反应速率的量子效应。具体目标包括更好地理解非Born-Oppenheimer效应、核量子效应以及反应性和能量处置中的模式特异性。与实验小组的合作将有助于指导计算研究，以便更好地理解固体表面上能量转移和化学转化的复杂相互作用。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。