Reaction Dynamics in Molecular Cluster Ions

分子簇离子的反应动力学

• 批准号: 9873742
• 负责人: Robert Parson
• 金额: $ 26.7万
• 依托单位: University of Colorado at Boulder
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 1999
• 资助国家: 美国
• 起止时间: 1999-01-01 至 2002-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9873742&HistoricalAwards=false
• 关键词: Reaction; Dynamics; Molecular; Cluster; Ions

Robert Parsons is supported by the Theoretical and Computational Chemistry Program to theoretically investigate complex dynamics in cluster ions. He uses clusters to discover the microscopic details of solvation, electron transfer, and energy dissipation that distinguish reactions in the condensed phase from their gas-phase analogs. Projects include molecular dynamics simulations of iodine anion photodissociation in carbonyl sulfide clusters, a more rigorous treatment of simulated time-resolved photoelectron spectra, and development of a kinetic theory of vibrational relaxation incorporating solvent evaporation.Molecular ions in the gas-phase can become solvated by surrounding neutral molecules in much the same way as ions become solvated by water in aqueous solutions. This research establishes connections to condensed phase phenomena by increasing our understanding of cluster dynamics. In particular, the role of strong and long-ranged solute-solvent interactions has not heretofore been investigated in detail. Parson's use of hierarchical models is particularly valuable in delineating the possible limitations of simpler descriptions of these phenomena.

罗伯特·帕森斯是由理论和计算化学计划支持的，从理论上研究团簇离子中的复杂动力学。他使用团簇来发现溶剂化、电子转移和能量耗散的微观细节，这些细节将凝聚相中的反应与其气相类似物区分开来。项目包括分子动力学模拟碘负离子在羰基硫化物团簇中的光解离，对模拟的时间分辨光电子光谱进行更严格的处理，以及开发包含溶剂挥发的振动弛豫动力学理论。气相中的分子离子可以被周围的中性分子溶剂化，就像离子在水溶液中被水溶剂化一样。这项研究通过增加我们对团簇动力学的理解，建立了与凝聚相现象的联系。特别是，到目前为止还没有详细研究过强的和长程的溶质-溶剂相互作用的作用。帕森对层次模型的使用在描述这些现象的更简单描述的可能局限性方面特别有价值。