Volume 113, 1999

The interaction of highly vibrationally excited molecules with surfaces: vibrational relaxation and reaction of NO(v) at Cu(111) and O/Cu(111)

Abstract

We have studied the reaction and inelastic scattering of ground and vibrationally excited NO on Cu(111). We employed laser-based techniques to prepare NO in vibrationally excited states, stimulated emission pumping (SEP) to prepare v=13 and v=15 and infrared overtone pumping to prepare v=2. Laser ionization detection schemes were developed for probing the state distribution of highly vibrationally excited NO molecules. Ground-state NO(v=0) dissociates at Cu(111) with a probability of ≈2×10-4, with little dependence on the translational energy in the range between 29 and 65 kJ mol-1. The dissociation probability is strongly enhanced by vibrational excitation to v=13 and 15. The dissociation continues until the oxygen coverage on Cu(111) reaches saturation. For highly excited NO(v=13, 15) scattering from O/Cu(111), we have seen efficient multi-quantum relaxation (up to Δv=-5). For NO(v=2), in contrast, the survival probability is nearly 90%. Measurements of the translational and rotational state distributions after scattering support a direct-inelastic mechanism for vibrational relaxation, with strong flow of energy into the surface. The branching ratios for vibrational relaxation are independent of the kinetic energy in our experiments.

Article information

Article type
Paper

Faraday Discuss., 1999,113, 181-199

The interaction of highly vibrationally excited molecules with surfaces: vibrational relaxation and reaction of NO(v) at Cu(111) and O/Cu(111)

H. Hou, C. T. Rettner, D. J. Auerbach, Y. Huang, S. J. Gulding and A. M. Wodtke, Faraday Discuss., 1999, 113, 181 DOI: 10.1039/A902660F

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