Quantum State-Resolved Studies of Chemisorption Reactions.

Quantum state-resolved gas/surface reaction dynamics probed by reflection absorption infrared spectroscopy.

We report the design and characterization of a new molecular-beam/surface-science apparatus for quantum state-resolved studies of gas/surface reaction dynamics combining optical state-specific reactant preparation in a molecular beam by rapid adiabatic passage with detection of surface-bound reaction products by reflection absorption infrared spectroscopy (RAIRS). RAIRS is a non-invasive infrar...

Quantum state resolved gas-surface reaction dynamics experiments: a tutorial review.

We present a tutorial review of our quantum state resolved experiments designed to study gas-surface reaction dynamics. The combination of a molecular beam, state specific reactant preparation by infrared laser pumping, and ultrahigh vacuum surface analysis techniques make it possible to study chemical reactivity at the gas-surface interface in unprecedented detail. We describe the experimental...

Rotational and steric effects in water dissociative chemisorption on Ni(111)

Powerful laser techniques have recently enabled quantum-state resolved molecular beam experiments for investigating gas-surface reactions, which have unveiled intriguing vibrational, rotational, and also steric effects. For reactions involving polyatomic molecules, e.g., the dissociative chemisorption of methane and water, the rotational and related steric effects are far less understood despit...

Quantum state-resolved CH4 dissociation on Pt(111): coverage dependent barrier heights from experiment and density functional theory.

The dissociative chemisorption of CH4 on Pt(111) was studied using quantum state-resolved methods at a surface temperature (T(s)) of 150 K where the nascent reaction products CH3(ads) and H(ads) are stable and accumulate on the surface. Most previous experimental studies of methane chemisorption on transition metal surfaces report only the initial sticking coefficients S0 on a clean surface. Re...

Energy Partitioning in Polyatomic Chemical Reactions: Quantum State Resolved Studies of Highly Exothermic Atom Abstraction Reactions from Molecules in the Gas Phase and at the Gas-Liquid Interface