Growth of crystalline Al2O3 via thermal atomic layer deposition: Nanomaterial phase stabilization

We report the growth of crystalline Al2O3 thin films deposited by thermal Atomic Layer Deposition (ALD) at 200 °C, which up to now has always resulted in the amorphous phase. The 5 nm thick films were deposited on Ga2O3, ZnO, and Si nanowire substrates 100 nm or less in diameter. The crystalline nature of the Al2O3 thin film coating was confirmed using Transmission Electron Microscopy (TEM), including high-resolution TEM lattice imaging, selected area diffraction, and energy filtered TEM. Al2O3 coatings on nanowires with diameters of 10 nm or less formed a fully crystalline phase, while those with diameters in the 20–25 nm range resulted in a partially crystalline coating, and those with diameters in excess of 50 nm were fully amorphous. We suggest that the amorphous Al2O3 phase becomes metastable with respect to a crystalline alumina polymorph, due to the nanometer size scale of the film/substrate combination. Since ALD Al2O3 films are widely used as protective barriers, dielectric layers, as well as potential coatings in energy materials, these findings may have important implications.