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Based on high resolution transmission electron microscopy, the primary orientational relationship at the Al/ Al2O3 interface has been observed to be one that matches the close packed planes and directions in the two phases17 In this orientation the Al(111) plane is parallel to the Al2O3(0001) basal plane and the following directions are parallel to each other:As is the case for other similar metal/Al2O3 interfaces2,34,35, the stoichiometry of clean Al/ Al2O3 interface is a function of the oxygen partial pressure. Previous first principles based analysis25 has suggested that the clean Al/Al2O3 interface can be stoichiometric, oxygen terminated, or aluminum terminated, depending on the ambient oxygen partial pressure. For the relatively low oxygen partial pressures36, usually associated with sessile drop experiments, the interface is predicted to be stoichiometric.