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

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.

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 Creators:
Bartels, C., Author
Golibrzuch, K., Author
Kandratsenka, A.1, Author           
Cooper, R., Author
Rahinov, I., Author
Auerbach, D. J.2, Author           
Wodtke, A. M.2, Author           
Affiliations:
1Research Group of Reaction Dynamics, MPI for biophysical chemistry, Max Planck Society, ou_578601              
2Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society, ou_578600              

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 Abstract: 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.

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Language(s): eng - English
 Dates: 2012-11-272012
 Publication Status: Issued
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1063/1.4769695
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Title: Molecular beams and molecular collisions. 28. International Symposium on Rarefied Gas Dynamics.
Source Genre: Proceedings
 Creator(s):
Mareschal, M., Editor
Santos, A., Editor
Affiliations:
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Publ. Info: Melville, N.Y. : American Institute of Physics
Pages: 10 Volume / Issue: 2 Sequence Number: - Start / End Page: 1330 - 1339 Identifier: ISBN: 978-0-7354-1115-9