Al Interaction with ZnO Surfaces
Résumé
Deposition of Al onto ZnO surfaces is important for metal/insulator contacts in microelectronics and photovoltaic devices, and also for nano-energetic materials; yet there have not been fundamental studies of these interfaces, in particular those involving the polar faces of ZnO. Density Functional calculations and Low Energy Ion Scattering (LEIS) studies are combined to unravel the chemistry of Al interaction on polar ZnO surfaces, revealing that Al atoms quasi spontaneously replace surface Zn atoms on both O-and Zn-terminated ZnO surfaces. In this process, aluminum atoms attract oxygen atoms, releasing zinc atoms through electrostatic repulsion within the growing alumina film. Kinetics and thermodynamics calculations indicate that zinc atoms accumulate on the surface rather than migrating into ZnO bulk at room temperature, due to high bulk diffusion barriers. Upon annealing to moderate temperatures, LEIS studies indicate that surface Zn atoms desorb at ~ 140-150 °C, which is consistent with the calculated 1.31 eV activation barrier.