Inter- and Intra-Molecular Dynamics of Highly Vibrationally Excited Molecules

在这个由化学系物理化学计划资助的项目中，宾夕法尼亚大学的戴海龙将继续进行一项关于高振动激发分子动力学的研究计划。这个项目将把关于非常高激发系统的详细松弛机制和速率的工作扩展到低温，并将研究在相同高振动能级的更广泛的动能区域内控制非弹性旋转过程的基本原理。第二组实验使用范德华络合物来研究从高振动激发的分子到附近的冷分子的能量转移，以深入了解不同的耦合机制、超级碰撞以及在固定能量激发的分子中的能量转移。动力学量子拍频光谱和时间分辨傅立叶变换发射光谱等技术将被用来关联这两种类型的实验的分子间和分子内相互作用。这项工作将有助于理解各种碰撞现象，如成核和低温反应动力学。因此，这项工作与社会关注的问题有关，如燃料的更有效燃烧和大气化学问题，如北极和南极臭氧空洞的形成和破坏。

In this project funded by the Physical Chemistry Program of the Chemistry Division, Hai-Lung Dai of the University of Pennsylvania will pursue a program of research on the dynamics of highly vibrationally excited molecules. This project will extend work on the detailed relaxation mechanisms and rates of very highly excited systems to low temperature and will investigate the underlying principles governing inelastic rovibrational processes across a broader kinetic energy regime of the same high vibrational level. A second set of experiments uses van der Waals complexes to study energy transfer from a highly vibrationally excited molecule to a nearby cold molecule to gain insight into different coupling mechanisms, super collisions, and energy transfer in molecules excited at fixed energies. Techniques such as kinetic quantum beat spectroscopy and time-resolved Fourier transform emission spectroscopy will be used to correlate the inter- and intra-molecular interactions for both types of experiment. This work will assist in understanding a wide variety of collisional phenomena, such as nucleation and low temperature reaction dynamics. As such, this work has relevance to societal concerns such as more efficient combustion of fuels and problems in atmospheric chemistry such as the formation and destruction of the Arctic and Antarctic ozone holes.