The angular distributions of NO photodesorbed from a Pt(111) surface by UV-
laser irradiation at 193 nm are investigated as a function of velocity usin
g a quantum state specific detection method, which combines resonance enhan
ced multiphoton ionization (REMPI) and a two-dimensional-imaging technique.
The angular distributions of NO in individual rovibrational states are obs
erved to be strongly peaked in the surface normal direction and are consist
ently reproduced by gaussian functions in the desorption angle theta. The a
ngular width of these distributions is found to decrease substantially with
the velocity of the desorbing molecules. The identical velocity dependence
of the angular distributions is observed independent of the rotational qua
ntum states of the photodesorbed NO molecules. This is indicative of a de-c
oupling of the rotational motion of the molecular axis and the hindered par
allel translation of the molecules in the adsorption ground state as well a
s in the excited states probed by the desorption process. The implications
of a simple impulsive model, which relates the amplitude of the frustrated
translational motion to the velocity dependence of the observed angular dis
tributions, are discussed. (C) 1999 Elsevier Science B.V. All rights reserv
ed.