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The dissociation of methane is not only an important reaction step in catalytic processes, but also of fundamental interest. Dynamical effects during the dissociative chemisorption of methane on metal surfaces cause significant differences in computed reaction rates, compared to what is predicted by typical transition state theory (TST) models. It is clear that for a good understanding of the catalytic activation of methane dynamical simulations are required. In this paper, a general blueprint is provided for performing dynamical simulations of the dissociative chemisorption of methane on metal surfaces, by employing either the quasi-classical trajectory or ring polymer molecular dynamics approach. If the computational setup is constructed with great care-since results can be affected considerably by the setup - chemically accurate predictions are achievable. Although this paper concerns methane dissociation, the provided blueprint is, so far, applicable to the dissociative chemisorption of most molecules. [ABSTRACT FROM AUTHOR]

Understanding the microscopic mechanism of molecule–surface interaction is of great importance in the study of chemical dynamics. Yet, it remains challenging to experimentally acquire quantum state resolved results, particularly the results related to different degrees of freedom of the reactants. Here, we report the design and performance of a new apparatus for molecule–surface dynamics studies, which enable the measurement of quantum state-resolved adsorption. A continuous narrow-linewidth infrared laser source and molecular beam unit were developed and employed in this new apparatus to achieve independent control on different degrees of freedom (translation, vibration, and rotation) of the molecule. Preliminary results on hydrogen and hydrogen chloride adsorption on the Cu (111) surface were also presented. [ABSTRACT FROM AUTHOR]