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 (n ∼ 1014 cm-2) and smaller electron effective mass (0.47me) than the later one (n ∼ 1013 cm-2, and 0.70me). 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.