Experimental & Theoretical Explorations of Reaction Dynamics at the Gas-Surface Interface 117 views

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

English

All rights reserved (no additional license for public reuse)

2023-12-06