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Volume 117, Issue 19, 15 November 2002
Surface reactivity of highly vibrationally excited molecules prepared by pulsed laser excitation: on Ni(100)117(2002); http://dx.doi.org/10.1063/1.1519860View Description Hide Description
We report state resolved sticking coefficients for highly vibrationally excited on Ni(100) at well-defined kinetic energies in the range of 12–72 kJ/mol. Incident methane molecules are prepared by pulsed laser radiation in single rovibrational levels of the first overtone of the antisymmetric stretch at and collided at normal incidence with a clean Ni(100) single crystal. We find that the vibrational excitation enhances the reaction probability by a factor 100 at an incident translational energy of 72 kJ/mol, but this enhancement increases to more than 4 orders of magnitude at low kinetic energy. Despite this large increase in the sticking coefficient, vibrational energy in appears to be about 80% as effective as an equivalent amount of translational energy in promoting the chemisorptionreaction.