Vibrational Dynamics: Weakly Bound Complexes and Molecule Surface Scattering

北卡罗来纳大学教堂山分校的罗杰·e·米勒（Roger E. Miller）得到了实验物理化学项目和多学科活动办公室的支持，继续他对弱结合配合物的状态-状态动力学的高分辨率红外研究。他将专注于水二聚体，这是理论化学界特别感兴趣的，并测量旋转和振动光碎片分布，标量和矢量相关性，以及解离能。在一项新的研究中，米勒将研究与单晶表面振动激发物质散射相关的分子间力和振动能量转移。这里的重点将放在实验方法的改进和更复杂的多原子分子的研究上。两个到几十个分子松散地结合在一起的分子簇可以被视为“孤立的”单个气体分子和组成固体的扩展分子阵列之间的中间阶段。了解这些团簇的行为有助于我们更好地理解从气体到固体转变的本质。事实上，团簇是相当普遍的，在大气化学中扮演着重要的角色，因此我们需要了解它们形成和破碎的动力学，以及组成团簇的分子之间的力的本质。对影响单个气体分子如何与“超星系团”或表面相互作用的力的研究的最新努力可以被视为米勒早期工作的简单扩展。

Roger E. Miller of the University of North Carolina at Chapel Hill is supported by the Experimental Physical Chemistry Program and the Office of Multidisciplinary Activities to continue his high resolution infrared studies on the state-to-state dynamics of weakly bound complexes. He will focus on the water dimer, which is of particular interest to the theoretical chemistry community, and measure the rotational and vibrational photofragment distributions, scalar and vector correlations, and dissociation energies. In a newer effort, Miller will investigate the intermolecular forces and vibrational energy transfer associated with the scattering of vibrationally excited species from single crystal surfaces. Emphasis here will be on improvements in experimental methods and the investigation of more complex, polyatomic molecules. Molecular clusters of two to tens of molecules loosely bound together can be viewed as the intermediary stage between `isolated` single gas molecules and the extended arrays of molecules that make up the solid. Understanding the behavior of such clusters helps us to better understand the nature of the transition from gas to solid. As it is, clusters are fairly ubiquitous and play important roles in atmospheric chemistry, thus we need to understand the dynamics of their formation and fragmentation, the nature of the forces between the molecules that make up the cluster. The newer effort on the study of the forces that influence how a single gas molecule interacts with a `supercluster` or surface can be viewed as a simple extension of the earlier work by Miller.