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This work explores the applicability of atomic layer deposition (ALD) in producing highly oriented crystalline gallium oxide films on foreign substrates at low thermal budgets. The effects of substrate, deposition temperature, and annealing process on formation of crystalline gallium oxide are discussed. The Ga 2 O 3 films exhibited a strong preferred orientation on the c-plane sapphire substrate. The onset of formation of crystalline gallium oxide is determined, at which only two sets of planes, i.e., α-Ga 2 O 3 (006) and β-Ga 2 O 3 (4̅ 02), are present parallel to the surface. More specifically, this work reports, for the first time, that epitaxial gallium oxide films on sapphire start to form at deposition temperatures ≥ 190 °C by using an optimized plasma-enhanced ALD process such that α-Ga 2 O 3 (006)∥α-Al 2 O 3 (006) and β-Ga 2 O 3 (2̅ 01)∥α-Al 2 O 3 (006). Both α-Ga 2 O 3 (006) and β-Ga 2 O 3 (2̅ 01) planes are polar planes (i.e., consisting of only one type of atom, either Ga or O) and, therefore, favorable to form by ALD at such low deposition temperatures. Ellipsometry and van der Pauw measurements confirmed that the crystalline films have optical and electrical properties close to bulk gallium oxide. The film grown at 277 °C was determined to have superior properties among as-deposited films. Using TEM to locate α-Ga 2 O 3 and β-Ga 2 O 3 domains in the as-deposited crystalline films, we proposed a short annealing scheme to limit the development of α-Ga 2 O 3 domains in the film and produce pure β-Ga 2 O 3 films via an energy-efficient process. A pure β-Ga 2 O 3 phase on sapphire with β-Ga 2 O 3 (2̅ 01)∥α-Al 2 O 3 (006) was successfully achieved by using the proposed process at the low annealing temperature of 550 °C preceded by the low deposition temperature of 190 °C. The results of this work enable epitaxial growth of gallium oxide thin films, with superior material properties offered by ALD, not only with potential applications as a high-performance material in reducing global energy consumption but also with an energyefficient fabrication process.

Metamaterials mediate long-range dipole-dipole interactions between quantum emitters.