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Buchkapitel

Vibrational excitation and relaxation of NO molecules scattered from a Au(111) surface.

MPG-Autoren
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Kandratsenka,  A.
Research Group of Reaction Dynamics, MPI for biophysical chemistry, Max Planck Society;

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Auerbach,  D. J.
Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society;

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Wodtke,  A. M.
Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society;

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Zitation

Bartels, C., Golibrzuch, K., Kandratsenka, A., Cooper, R., Rahinov, I., Auerbach, D. J., et al. (2012). Vibrational excitation and relaxation of NO molecules scattered from a Au(111) surface. In M. Mareschal, & A. Santos (Eds.), Molecular beams and molecular collisions. 28. International Symposium on Rarefied Gas Dynamics. (pp. 1330-1339). Melville, N.Y.: American Institute of Physics. doi:10.1063/1.4769695.


Zitierlink: http://hdl.handle.net/11858/00-001M-0000-000E-E80C-5
Zusammenfassung
We present results of recent and ongoing experiments on molecular-beam surface scattering of NO molecules from a Au(lll) surface. Vibrational excitation of NO(ν=0) into ν=l,2 was studied in great detail over a wide range of incidence energies (0.10-1.05 eV) and surface temperatures (300-1100 K). We find behavior characteristic of electronically nonadiabatic coupling of molecular vibration to electron-hole pair excitation in the gold crystal. A state-to-state kinetic model shows that for ν=2 excitation both the sequential (0→1→2) and direct (0→2) excitation pathways are important. The absolute excitation probabilities are also compared to the results of a first principles independent-electron surface hopping calculation, and good agreement is obtained. In addition to ν=l,2 excitation, we present the first evidence for second-overtone ν=3 vibrational excitation. Preliminary data for vibrational relaxation of laser-prepared NO(ν=3) show strong relaxation; the intrinsic coupling strengths are consistent with those obtained from vibrational excitation. Measurements of the translational inelasticity of NO(ν=3) show that the molecules lose a large fraction of translational energy in the collision. The translation-vibration coupling is significant but may depend on incidence energy, and a clear anticorrelation is observed between the final translational and rotational energies.