Abstract
The interaction of ammonia with ordered Pt surface was studies by means of surface core-level photoemission and tight-binding-type calculations. Clean Pt surfaces have distinguishable surface and bulk components of the 4f 7/2 core level. The 4f 7/2 surface component is shifted to lower binding energy (-0.32 eV) than the bulk on the clean (111) surface, but in the presence of ammonia the surface peak is shifted to positive binding energy (0.7 eV). This result is unexpected, since it indicates a depletion of d-electron density on Pt atoms attached to NH 3, in contrast to common assumptions of NH 3 as a net donor. Thin-film calculations show this depletion in the form of rehybridization of sp with d electrons on the Pt atom. The mixing of p z orbitals with the d band leads to a dipole moment perpendicular to the surface, which in addition to the static dipole of ammonia is also a major factor in the decrease in work function upon chemisorption.
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