Unimolecular Reaction Dynamics

这项研究是实验物理化学计划的一部分，旨在研究简单原型分子在解离阈值附近的光谱和动力学。这项研究的目的是了解当分子沿着解离路径进行时，分子振动和旋转的各种相互作用。将进行全态分辨实验，以观察分子在离解阈值下的光谱，测量单个量子态的离解率，并在乘积自由度之间映射能量和角动量的释放。这项研究的一个目的是确定当分子沿着反应坐标向解离产物前进时，振动和旋转自由度之间的耦合程度。所获得的数据应该为单分子反应的替代动力学模型提供强有力的检验。从头算势面将与最先进的动力学方法一起使用来比较理论和实验，这些方法提供了完全的能态光谱分辨率。

This research, part of the Experimental Physical Chemistry Program, is designed to study the spectroscopy and dynamics of simple prototypical molecules near their dissociation thresholds. The object of this study is to understand the interaction of the variety of molecular vibrations and rotations as a molecule proceeds along the path to dissociation. Fully state-resolved experiments will be done to observe the spectra of molecules at the threshold of dissociation, to measure dissociation rates for individual quantum states and to map the release of energy and angular momentum among product degrees of freedom. An aim of the study is to establish the extent of coupling between vibrational and rotational degrees of freedom as a molecule proceeds along the reaction coordinate to dissociation products. The data obtained should provide a strong test of alternative dynamical models of unimolecular reactions. Ab-initio potential surfaces will be used with state-of-the-art dynamical methods to compare theory and experiment which provide complete energy state spectral resolution.