Molecular beams have been used to search for evidence for a weakly bound molecular precursor in the interaction of O2 with Al(111). The experiments are consistent with a precursor whose binding energy is smaller than 0.1 eV. The total reflectivity as a function of incidence angle shows a pronounced dip at 25° for Etrans between 90 and 300 meV. This feature corroborates an earlier observation by Österlund et al. in sticking measurements. Modeling using a reduced dimensionality potential energy surface shows a similar behavior which is caused by steering into a shallow molecular adsorption well located at the same site in the unit cell as the maximum in the barrier towards dissociative adsorption. This effect is not observed if the molecular adsorption well is located at the same site as the minimum energy pathway to dissociative adsorption.
Experimental results are presented for the scattering of well-defined beams of molecular oxygen incident on clean Al(111). The data consist of scattered angular distributions measured as a function of incident angle, and for fixed incident angle, the dependence on surface temperature of the angular distributions. The measurements are interpreted in terms of a scattering theory that treats the exchange of energy between the translational and rotational motions of the molecule and the phonons of the surface using classical dynamics. The dependence of the measured angular distributions on incident beam angle and temperature is well explained by the theory. Rotational excitation and quantum excitation of the O(2) internal stretching mode are briefly discussed.
The surface photochemistry of NO(2) on ultrathin Ag(111) films (5-60 nm) on Si(100) substrates has been studied. NO(2), forming N(2)O(4) on the surface, dissociates to release NO and NO(2) into the gas phase with translational energies exceeding the equivalent of the sample temperature. An increase of the photodesorption cross section is observed for 266 nm light when the film thickness is decreased below 30 nm despite the fact that the optical absorptivity decreases. For 4.4 nm film thickness this increase is about threefold. The data are consistent with a similar effect for 355 nm light. The reduced film thickness has no significant influence on the average translation energy of the desorbing molecules or the branching into the different channels. The increased photodesorption cross section is interpreted to result from photon absorption in the Si substrate producing electrons with no or little momenta parallel to the surface at energies where this is not allowed in Ag. It is suggested that these electrons penetrate through the Ag film despite the gap in the surface projected band structure.
The surface photochemistry of on ultrathin epitaxial Ag films on Si(100) substrates has been studied with the goal to employ it as a tool to unravel the electron dynamics in such films. An increase of the photodesorption cross section is observed--a factor of 5 for 266 nm light and 12 nm film thickness--when the film thickness is decreased, despite the fact that the optical absorbtivity decreases. The increased photodesorption cross section is interpreted to result from photon absorption in the Si substrate producing electrons at energies and parallel momenta which are not allowed in Ag. These electrons penetrate through the Ag film despite the gap in the surface projected band structure utilizing quantum resonances.
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