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: 2019
• 资助国家: 加拿大
• 起止时间: 2019-01-01 至 2020-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=690480
• 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）光谱的最新进展，现在可以实时详细观察分子系统和化学反应，人们对化学反应动力学和热力学的理论研究越来越越来越多，可以预测，解释，解释和指导实验。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，从而提供有关化学反应机制和动力学的宝贵信息。这些研究是必不可少的，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，实验性可观察物质太复杂了，无法在没有理论的帮助下进行解释和理解。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。向新的方向提出了针对现实计算机模拟的工具的开发，其中包括对分子相互作用的改进描述以及对量子核效应的描述以及对量子核效应的包含和可能的非添加效应和可能的无效效应。大多数应用将集中在簇上，簇是原子或分子的聚集体，它们弥合了气体和凝结（液体）相之间的间隙。簇可以用作选择性微覆盖的工具，也可以是具有独特属性的不同类别的材料。我们将研究尤其是（1）簇纳米材料的结构和反应，（2）由离子和盐播种的溶剂簇的光化学，以及（3）复合离子和盐的簇和大量溶剂化。我们的理论研究将有助于解释和指导实验研究，并将有助于更深入的分子水平对化学的理解，并从纳米技术（例如氢/能量储存，催化）到生物学（例如蛋白质变性），并具有不同的潜在应用。