Abstract

Well-characterized Al(111) and Al(100) samples were studied with monoenergetic positrons before and after exposure to oxygen. Both positronium-formation and positron-emission curves were obtained for various incident positron energies at sample temperatures ranging from 160-900 K. The orthopositronium decay signal provides a unique signature that the positron has emerged from the surface region of a clean metal. In the clean Al crystals part of the positronium formed near the surface is found to be associated with a temperature-activated process described as the thermally activated detrapping of a positron from a surface state. A simple positron diffusion model, including surface and vacancy trapping, is fitted to the positronium data and an estimate of the binding energy of the positron in this trap is made. The positron diffusion constant is found to have a negative temperature dependence before the onset of positron trapping at thermally generated monovacancies (>500 K), in reasonable agreement with theoretical predictions. The depth of the positron surface state is reduced or positronium is formed in the chemisorbed layer as oxygen is adsorbed on both Al sample surfaces, thus increasing the positronium fraction and decreasing the positron emission. At higher oxygen exposures [>500 L (1 L = ${10}^{\ensuremath{-}6}$ torr sec)] positron or positronium traps are generated in the overlayer and the positronium fraction is reduced. The amorphous-to-crystalline surface transition of ${\mathrm{Al}}_{x}{\mathrm{O}}_{y}$ on Al is observed between 650 and 800 K by the change in the positronium fraction and is interpreted as the removal of trapping centers in the metal-oxide overlayer. At the higher temperatures and incident energies vacancy trapping is observed by the decrease in the positron diffusion length in both the clean and the underlying Al of the oxygen-exposed samples. Similar vacancy formation enthalpies for Al are extracted in both the clean and oxygen-covered samples by a simple model and are in good agreement with those measured by other experimental methods. This technique provides a new experimental means for the study of interfaces and thin films and the vacancy-type defects associated with them.

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