Gas-Phase Molecular Dynamics

The Gas-Phase Molecular Dynamics Program explores the energetics, dynamics and kinetics of chemical reactions resulting from molecular collisions in the gas phase. The goal of this work is a fundamental understanding of chemical processes related to combustion. We are interested in the microscopic factors affecting the structure, dynamics and reactivity of short-lived intermediates such as free radicals in gas-phase reactions. Molecular species are studied using both experimental and theoretical tools including high-resolution spectroscopic probes, velocity map imaging, time-of-flight mass spectrometry, ab initio electronic structure calculations and both time-dependent and time-independent quantum calculations of nuclear motion. The focus of the program has recently been broadened to include aspects of the chemical physics of catalysis, specifically chemical dynamics and kinetics at surfaces and on metal and metal-containing clusters, and the spectroscopy of metal-containing clusters. The synergy between the experimental and theoretical parts of the program cannot be overemphasized.

Two coupled large-amplitude vibrational coordinates for [HO-H-OH]^-, representing H transfer in a double well, with the barrier strongly dependent on the O-O distance. See H.-G. Yu, "A rigorous full-dimensional quantum dynamics calculation of the vibrational energies of H₃O₂^-" J. Chem. Phys. 125, 204306 (2006).