Theoretical Studies of Molecular Interactions, Structure, Dynamics and Spectroscopy in Clusters and Condensed Matter

团簇和凝聚态分子相互作用、结构、动力学和光谱学的理论研究

• 批准号: 216940-2013
• 负责人: Peslherbe, Gilles
• 金额: $ 3.93万
• 依托单位: Concordia University
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2018
• 资助国家: 加拿大
• 起止时间: 2018-01-01 至 2019-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=662016
• 关键词: Theoretical; Studies; Molecular; Interactions; Structure

With the recent advances in (ultrafast) spectroscopy, which now permit the observation of molecular systems in great detail and chemical reactions in real time, there is an ever increasing interest in theoretical studies of chemical reaction dynamics and thermodynamics, as they can predict, explain and guide experiments. In particular, molecular dynamics techniques allow the motion of atoms and molecules to be simulated at the microscopic level, providing invaluable information about the mechanism and kinetics of chemical reactions. These studies are essential since they provide a link between potential energy surfaces calculated by electronic structure theory (quantum chemistry) and experimental measurements of chemical dynamics and thermodynamics. In many instances, experimental observables are too convoluted to explain and understand without the help of theory. Furthermore, connection with experiment is crucial for assessing the reliability of computer simulations and theoretical models, which, in turn can be used to improve our fundamental understanding of chemistry.**New directions are proposed for the development of tools aimed at realistic computer simulations, which include an improved description of molecular interactions and the inclusion of quantum nuclear effects and possible nonadiabatic effects in dynamical simulations. Most applications will focus on clusters, which are aggregates of atoms or molecules which bridge the gap between the gas and condensed (liquid) phases. Clusters can be used as tools for selective microsolvation, or they can be a distinct class of materials with unique properties. We will study, in particular, (1) the structure and reactions of cluster nanomaterials, (2) the photochemistry of solvent clusters seeded by ions and salts, and (3) the cluster and bulk solvation of complex ions and salts. Our theoretical studies will help explain and guide experimental studies, and will contribute to a deeper molecular-level understanding of chemistry, with diverse potential applications from nanotechnology (e.g. hydrogen/energy storage, catalysis) to biology (e.g. protein denaturation).

随着（超快）光谱学的最新进展，现在可以非常详细地观察分子系统和实时化学反应，人们对化学反应动力学和热力学的理论研究越来越感兴趣，因为它们可以预测、解释并指导实验。特别是，分子动力学技术允许在微观水平上模拟原子和分子的运动，提供有关化学反应机制和动力学的宝贵信息。这些研究至关重要，因为它们提供了通过电子结构理论（量子化学）计算的势能表面与化学动力学和热力学的实验测量之间的联系。在许多情况下，实验观察结果过于复杂，如果没有理论的帮助就无法解释和理解。此外，与实验的联系对于评估计算机模拟和理论模型的可靠性至关重要，这反过来又可以用来提高我们对化学的基本理解。**为开发针对实际计算机模拟的工具提出了新的方向，其中包括对分子相互作用的改进描述以及在动力学模拟中纳入量子核效应和可能的非绝热效应。大多数应用将集中在团簇上，团簇是原子或分子的聚集体，弥合了气相和凝聚（液体）相之间的间隙。簇可以用作选择性微溶剂化的工具，或者它们可以是具有独特性质的一类独特材料。我们将特别研究（1）簇纳米材料的结构和反应，（2）离子和盐种子溶剂簇的光化学，以及（3）复杂离子和盐的簇和本体溶剂化。我们的理论研究将有助于解释和指导实验研究，并将有助于在分子水平上更深入地理解化学，以及从纳米技术（例如氢/能量存储、催化）到生物学（例如蛋白质变性）的各种潜在应用。