Oxide materials at the two-dimensional limit

Emergent phenomena in transition metal oxide films are receiving considerable attention with the development of techniques for the preparation of well-controlled oxide surfaces. On the macroscopic scale, such display novel physics phenomena including superconductivity, magnetism, ferroelectricity, and more. On the nanometer scale, the properties of epitaxial interfaces are further impacted by strain, band alignment, and crystal imperfections that may affect the long-range as well as the short-range order. Furthermore, symmetry lowering at the interface creates entirely new environments that are not accessible in the bulk environment. Thus, thin-film oxide materials are increasingly important in many applications. My work focuses on epitaxial oxides of the perovskite, spinel, and rocksalt structure and covers two main phenomena: (1) the two-dimensional electron gas at epitaxial oxide interfaces, and (2) thin epitaxial electro-optic oxides. Because polar oxides are of prominent interest as a mechanism for the formation of the two-dimensional electron gas, I start with a study of polar semiconductor Co₃O₄. Ellipsometry reveals a direct band gap of 0.75 eV, and magnetic measurements show the signature of antiferromagnetic ordering at 49 K, higher than the typical bulk value. Next, I look closer at the role of defects by studying the highly conducting layer at the crystalline [gamma]-alumina/SrTiO₃ (STO) interface which is attributed to oxygen vacancies. Annealing in oxygen is found to reduce the carrier density and turn a conductive sample into an insulator. Building upon these results, I show that even at room temperature, out-diffusion of oxygen from SrTiO₃ during epitaxy of highly spin-split semiconductor EuO epitaxy creates a highly conductive layer of oxygen vacancies on the SrTiO₃ side of the interface. The films are ferromagnetic with a Curie temperature of 70 K and display giant magnetoresistance below the transition temperature. Leveraging this approach offers an as-yet unexplored route to seamlessly integrate ferromagnetism and the oxide two-dimensional electron gas for the development of novel nano-oxide spintronic devices. The large effective Pockels coefficient for high-quality epitaxial BaTiO₃ (BTO) films on Si distinguishes BaTiO₃ as a highly promising material for integrated silicon nanophotonics. However, the linear electro-optic effect in BaTiO₃ thin films determined in previous experiments clearly shows deteriorated properties compared to bulk BTO crystals. First, I study BaTiO₃ films of varied thickness in order to quantify the Pockels coefficient with respect to crystalline orientation. As a next step, I report on the strong dependence of the Pockels effect in BaTiO₃ thin films on their microstructure, and provide guidelines on how to engineer thin films with strong electro-optic response. The 25× enhancement of the Pockels coefficient indicates a promising route to increase the performance of nonlinear oxides in the two-dimensional limit for the development of novel hybrid silicon photonic platform.