Dimensional control of defect dynamics in perovskite oxide superlattices

Successful modern generalized gradient approximations (GGA's) are biased toward atomic energies. Restoration of the first-principles gradient expansion for exchange over a wide range of density gradients eliminates this bias. We introduce PBEsol, a revised Perdew-Burke-Ernzerhof GGA that improves equilibrium properties of densely-packed solids and their surfaces.

The electronic reconstruction at the interface between two insulating oxides can give rise to a highly-conductive interface. In analogy to this remarkable interface-induced conductivity we show how, additionally, magnetism can be induced at the interface between the otherwise nonmagnetic insulating perovskites SrTiO3 and LaAlO3. A large negative magnetoresistance of the interface is found, together with a logarithmic temperature dependence of the sheet resistance. At low temperatures, the sheet resistance reveals magnetic hysteresis. Magnetic ordering is a key issue in solid-state science and its underlying mechanisms are still the subject of intense research. In particular, the interplay between localized magnetic moments and the spin of itinerant conduction electrons in a solid gives rise to intriguing many-body effects such as Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions, the Kondo effect, and carrier-induced ferromagnetism in diluted magnetic semiconductors. The conducting oxide interface now provides a versatile system to induce and manipulate magnetic moments in otherwise nonmagnetic materials.

A central goal of modern materials physics and nanoscience is control of materials and their interfaces to atomic dimensions. For interfaces between polar and non-polar layers, this goal is thwarted by a polar catastrophe that forces an interfacial reconstruction. In traditional semiconductors this reconstruction is achieved by an atomic disordering and stoichiometry change at the interface, but in multivalent oxides a new option is available: if the electrons can move, the atoms don`t have to. Using atomic-scale electron energy loss spectroscopy we find that there is a fundamental asymmetry between ionically and electronically compensated interfaces, both in interfacial sharpness and carrier density. This suggests a general strategy to design sharp interfaces, remove interfacial screening charges, control the band offset, and hence dramatically improving the performance of oxide devices.