Mica single crystal (001) surfaces are irradiated with light from an excimer laser (λ=248 nm) and are analyzed via low‐energy electron diffraction. It is shown that the excimer laser treatment makes them well suited for epitaxial growth of Au(111) thin films (thickness 150–600 Å). Further irradiation with the laser at reduced fluences improves the quality of the grown Au films significantly without the need for high‐energy ion sputtering.

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