MeV He+ ion scattering/channeling (HEIS), angle resolved XPS, and RHEED have been applied to study the Au and MBE‐grown GaAs(001)‐c(4×4) interface structures in the Au film thickness range of ≲70 Å and the annealing temperature range from room temperature up to ∼300 °C. The results show release of the As atoms and epitaxial growth of the Au film even at room temperature. The shrinked Au film after annealing displays selective registry to the [1̄10] direction, which is believed to result from a strong Au–GaAs(001) interaction.

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