Comparison Studies of Interfacial Electronic and Energetic Properties of LaAlO₃/TiO₂ and TiO₂/LaAlO₃ Heterostructures from First-Principles Calculations

By using first-principles electronic structure calculations, we studied electronic and energetic properties of perovskite oxide heterostructures with different epitaxial growth order between anatase TiO₂ and LaAlO₃. Two types of heterostructures, i.e., TiO₂ film grown on LaAlO₃ substrate (TiO₂/LaAlO₃) and LaAlO₃ film grown on TiO₂ substrate (LaAlO₃/TiO₂), were modeled. The TiO₂/LaAlO₃ model is intrinsically metallic and thus does not exhibit an insulator-to-metal transition as TiO₂ film thickness increases; in contrast, the LaAlO₃/TiO₂ model shows an insulator-to-metal transition as the LaAlO₃ film thickness increases up to 4 unit cells. The former model has a larger interfacial charge carrier density (<i>n</i> ∼ 10¹⁴ cm^–2) and smaller electron effective mass (0.47<i>m</i>_e) than the later one (<i>n</i> ∼ 10¹³ cm^–2, and 0.70<i>m</i>_e). The interfacial energetics calculations indicate that the TiO₂/LaAlO₃ model is energetically more favorable than the LaAlO₃/TiO₂ model, and the former has a stronger interface cohesion than the later model. This research provides fundamental insights into the different interfacial electronic and energetic properties of TiO₂/LaAlO₃ and LaAlO₃/TiO₂ heterostructures