AVS 49th International Symposium
    Surface Science Tuesday Sessions
       Session SS1-TuA

Paper SS1-TuA5
On the Detection of Chemically-Induced Hot Electrons in Surface Processes: from X-ray Edges to Schottky Barriers

Tuesday, November 5, 2002, 3:20 pm, Room C-108

Session: Ultrafast Phenomena & Dynamics at Surfaces
Presenter: J.W. Gadzuk, National Institute of Standards and Technology
Correspondent: Click to Email

The potential involvement of electron-hole pair excitations in atomic/molecular processes such as sticking/adsorption/dissociation at metal surfaces has long been debated, particularly by those previously involved with similar issues in electron spectroscopies of localized core levels in solids. Of special relevance here are the fundamental studies of Müller-Hartmann et al.@footnote 1@ on the dynamic response of Fermi systems to transient localized perturbations as subsequently applied to problems in non-adiabatic surface dynamics.@footnote 2@ Recent experiments have detected hot electrons produced when various gases were adsorbed on a thin metal film that formed a Schottky barrier with an n-type Si substrate upon which the film was deposited.@footnote 3@ Drawing on analogies with electron-hole pair shakeup in spectroscopic processes which lead to the x-ray edge singularity, a theoretical model for the electronically non-adiabatic effects is presented here that accounts for the observed initial hot electron production, roughly 10@super -3@-10@super -2@electrons per incident strongly-interacting adsorbate such as O, H, and NO@sub 2@ on Ag. Since the fundamental physical content of the x-ray edge model is the Fermi-level phase shift associated with the localized perturbation and the rate at which it is switched on, straightforward connections with friction-based models@footnote 4@ are easily established in an intuitively satisfying way. @FootnoteText@ @footnote 1@E. Müller-Hartmann, T. V. Ramakrishnan, and G. Toulouse, Phys.Rev.B 3,1102(1971). @footnote 2@J. W. Gadzuk and H. Metiu, Phys.Rev.B 22,2603(1980); ibid. 24,1866(1981). @footnote 3@B. Gergen, H. Nienhaus, W. H. Weinberg, and E. W. McFarland, Science 294,2521(2001); H. Nienhaus, Surface Sci. Repts. 45,1(2002). @footnote 4@K. Schönhammer and O. Gunnarsson, Phys. Rev.B 27,5113(1983).