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Evidence for coupled rotational and phonon quantum excitation in the scattering of a nearly monoenergetic HD beam from the Ni(001) surface

Journal Article · · Journal of Chemical Physics; (USA)
DOI:https://doi.org/10.1063/1.458105· OSTI ID:7021660
; ;  [1]
  1. Max-Planck-Institut f uer Stroemungsforschung, Bunsenstrasse 10, 3400 Goettingen, Federal Republic of Germany (DE)
Angular distributions and time-of-flight spectra of a nearly monoenergetic ({Delta}{ital v}/{ital v}{congruent}2% FWHM) He seeded HD beam ({ital k}{sub {ital i}}=6.80 A{sup {minus}1}, {ital E}{sub {ital i}}=32 meV) have been measured after scattering from a Ni(001) single-crystal surface along the {l angle}100{r angle} azimuth. The most intense peaks in the angular distributions are attributed to diffraction with rotational excitation while the rotationally elastic diffraction peaks are an order of magnitude smaller. All the time-of-flight distributions reveal intense peaks at {Delta}{ital E}={minus}11.06 meV corresponding to the HD rotational transition {ital j}{sub {ital i}}=0{r arrow}{ital j}{sub {ital f}}=1. The rotational energy loss observed at angles between the diffraction peaks is attributed to incoherent inelastic scattering at defects. The other inelastic peaks in the time-of-flight spectra can be assigned to phonons which are created or annihilated in the rotationally inelastic collisions. The measured phonon dispersion curves suggest a predominant interaction with the transverse bulk edge and not with the Rayleigh mode. These results provide the first direct evidence for a coupling of rotational transitions to the phonons of a metal surface. The pronounced rotational inelasticity at step edges does not support the widely held view that nonactivated chemisorption occurs at step edges.
OSTI ID:
7021660
Journal Information:
Journal of Chemical Physics; (USA), Journal Name: Journal of Chemical Physics; (USA) Vol. 92:2; ISSN JCPSA; ISSN 0021-9606
Country of Publication:
United States
Language:
English