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Atomic layer deposition (ALD) is an essential tool in semiconductor devicefabrication that allows the growth of ultrathin and conformal films toprecisely form heterostructures and tune interface properties. Theself-limiting nature of the chemical reactions during ALD provides excellentcontrol over the layer thickness. However, in contrast to idealized growthmodels, it is experimentally challenging to create continuous monolayers by ALDbecause surface inhomogeneities and precursor steric interactions result inisland growth during film nucleation. Thus, the ability to create pin-hole freemonolayers by ALD would offer new opportunities for controlling interfacialcharge and mass transport in semiconductor devices, as well as for tailoringsurface chemistry. Here, we report full encapsulation of c-plane galliumnitride (GaN) with an ultimately thin (~3 {\AA}) aluminum oxide (AlOx)monolayer, which is enabled by the partial conversion of the GaN surface oxideinto AlOx using a combination of trimethylaluminum deposition and hydrogenplasma exposure. Introduction of monolayer AlOx significantly modifies thephysical and chemical properties of the surface, decreasing the work functionand introducing new chemical reactivity to the GaN surface. This tunableinterfacial chemistry is highlighted by the reactivity of the modified surfacewith phosphonic acids under standard conditions, which results inself-assembled monolayers with densities approaching the theoretical limit.More broadly, the presented monolayer AlOx deposition scheme can be extended toother dielectrics and III-V-based semiconductors, with significant relevancefor applications in optoelectronics, chemical sensing, and(photo)electrocatalysis.

Aluminum Oxide at the Monolayer Limit via Oxidant-free Plasma-Assisted Atomic Layer Deposition on GaN