A method of depositing a hafnium-based dielectric film is provided. The method comprises atomic layer deposition using ozone and one or more reactants comprising a hafnium precursor. A semiconductor device is also provided. The device comprises a substrate, a hafnium-based dielectric layer formed atop the substrate, and an interfacial layer formed between the substrate and the hafnium-based dielectric layer, wherein the interfacial layer comprises silicon dioxide and has a crystalline structure.