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

Christof Bartels, Kai Golibrzuch, Alexander Kandratsenka, Russell Cooper, Igor Rahinov, Daniel J. Auerbach, Alec M. Wodtke

Research output: Chapter in Book/Report/Conference proceedingConference contributionpeer-review


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.

Original languageEnglish
Title of host publication28th International Symposium on Rarefied Gas Dynamics 2012
Number of pages10
StatePublished - 2012
Event28th International Symposium on Rarefied Gas Dynamics 2012, RGD 2012 - Zaragoza, Spain
Duration: 9 Jul 201213 Jul 2012

Publication series

NameAIP Conference Proceedings
ISSN (Print)0094-243X
ISSN (Electronic)1551-7616


Conference28th International Symposium on Rarefied Gas Dynamics 2012, RGD 2012


  • Molecular beams
  • independent-electron surface hopping
  • nonadiabatic dynamics
  • surface chemistry


Dive into the research topics of 'Vibrational excitation and relaxation of NO molecules scattered from a Au(111) surface'. Together they form a unique fingerprint.

Cite this