Experimental & Theoretical Explorations of Reaction Dynamics at the Gas-Surface Interface

Bernard, Mark, Chemistry - Graduate School of Arts and Sciences, University of Virginia
Harrison, Allan, AS-Chemistry (CHEM), University of Virginia
Lehmann, Kevin, AS-Chemistry (CHEM), University of Virginia

The dynamics of gas-surface interactions, both physical and chemical, are investigated for a series of small molecules on transition metal surfaces. Investigations begin by quantifying the propensity for the vibrationally-activated photodesorption of surface-bound methane on Pt(111) using a tunable infrared light source. A statistical precursor mediated microcanonical trapping (s-PMMT) model and its dynamically biased variant (d-PMMT) are used to assess the dynamics of dissociative chemisorption and to extract transition state properties from experimental data. PMMT models are discussed for analyzing and simulating both non-equilibrium and equilibrium experiments for the dissociative chemisorption of HCl on Au(111), methane (CH4) on Pt(111), and neopentane (2,2-dimethylpropane) on Pt(111). Finally, the capacity to measure trapping and dissociative sticking coefficients using laser-induced thermal techniques is discussed as it relates to the CH4/Pt(111) system.

PHD (Doctor of Philosophy)
Heterogeneous Catalysis, Chemical Physics, Chemical Dynamics, Surface Science
Sponsoring Agency:
National Science Foundation
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