Synthesis of Model Al-Al2O3 Multilayer Systems with Monolayer Oxide Thickness Control by Circumventing Native Oxidation

•Physical vapor deposition and atomic layer deposition systems were integrated.•The sample was transferred within deposition chambers without breaking high vacuum.•An Al-Al2O3 multilayer brick-mortar structure was deposited by the hybrid system.•Each ultrathin Al2O3 sublayer interrupted the grain growth of the Al sublayer.•Surface oxidation of Al sublayers was circumvented by keeping sample in high vacuum.