Oxide heterostructures have been shown to exhibit unusual physics and hold the promise of novel electronic applications. We present a set of criteria to select and design interfaces, particularly those that can sustain a high-density twodimensional electron gas (2DEG). We describe how first-principles calculations can contribute to a qualitative and quantitative understanding, illustrated with the key issue of band alignment. Band offsets determine on which side of the interface the 2DEG will reside, as well as the degree of confinement. We use hybrid density functional calculations to determine the band alignments of a number of complex oxides, considering materials with different types of conduction-band character, polar or nonpolar character and band insulators as well as Mott insulators. We suggest promising materials combinations that could lead to a 2DEG with optimized properties, such as high 2DEG densities and high electron mobilities.

The polar discontinuity at the SrTiO 3 /LaAlO 3 interface (STO/LAO) can in principle sustain an electron density of 3.3×10 14 cm −2 (0.5 electrons per unit cell). However, experimentally observed densities are more than an order of magnitude lower. Using a combination of first-principles and Schrödinger-Poisson simulations we show that the problem lies in the asymmetric nature of the structure, i.e., the inability to form a second LAO/STO interface that is a mirror image of the first, or to fully passivate the LAO surface. Our insights apply to oxide interfaces in general, explaining for instance why the SrTiO 3 /GdTiO 3 interface has been found to exhibit the full density of 3.3×10 14 cm −2 .

BaSnO3 (BSO) is a transparent perovskite oxide with high room-temperature mobility, a property that is highly desirable for a channel material in transistors. However, its low density of states (DOS) makes it challenging to confine a high-density two-dimensional electron gas (2DEG). Using hybrid density functional theory, we calculate the band structure of BSO, its DOS, and its band offsets with candidate barrier materials, such as SrTiO3 (STO), LaInO3, and KTaO3. With the calculated material parameters as input, Schrödinger-Poisson simulations are then performed on BSO heterostructures to quantitatively address the issue of 2DEG confinement. The BSO/STO interface with a conduction-band offset of 1.14 eV limits the 2DEG density confined within BSO to 8×1013 cm−2. Strategies to improve the confinement via band-offset engineering are discussed.

A complete structural solution of the bilayer iridate compound Sr3Ir2O7 presently remains outstanding. Previously reported structures for this compound vary and all fail to explain weak structural violations observed in neutron scattering measurements as well as the presence of a net ferromagnetic moment in the basal plane. In this paper, we present single crystal neutron diffraction and rotational anisotropy second harmonic generation measurements unveiling a lower, monoclinic symmetry inherent to Sr3Ir2O7. Combined with density functional theory, our measurements identify the correct structural space group as No. 15 (C2/c) and provide clarity regarding the local symmetry of Ir 4+ cations within this spin-orbit Mott material.

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The interfaces between two condensed phases often exhibit emergent physical properties that can lead to new physics and novel device applications and are the subject of intense study in many disciplines. We here apply experimental and theoretical techniques to the characterization of one such interesting interface system: the two-dimensional electron gas (2DEG) formed in multilayers consisting of SrTiO 3 (STO) and GdTiO 3 (GTO). This system has been the subject of multiple studies recently and shown to exhibit very high carrier charge densities and ferromagnetic effects, among other intriguing properties. We have studied a 2DEG-forming multilayer of the form [6 unit cells (u.c.) STO/3 u.c. of GTO] 20 using a unique array of photoemission techniques including soft and hard x-ray excitation, soft x-ray angle-resolved photoemission, core-level spectroscopy, resonant excitation, and standing-wave effects, as well as theoretical calculations of the electronic structure at several levels and of the actual photoemission process. Standing-wave measurements below and above a strong resonance have been exploited as a powerful method for studying the 2DEG depth distribution. We have thus characterized the spatial and momentum properties of this 2DEG in detail, determining via depth-distribution measurements that it is spread throughout the 6 u.c. layer of STO and measuring the momentum dispersion of its states. The experimental results are supported in several ways by theory, leading to a much more complete picture of the nature of this 2DEG and suggesting that oxygen vacancies are not the origin of it. Similar multitechnique photoemission studies of such states at buried interfaces, combined with comparable theory, will be a very fruitful future approach for exploring and modifying the fascinating world of buried-interface physics and chemistry.

The perovskite stannates (ASnO3; A = Ba, Sr, Ca) are promising for oxide electronics, but control of n-type doping has proved challenging. Using first-principles hybrid density functional calculations, we investigate La dopants and explore the formation of compensating acceptor defects. We find that La on the A site always behaves as a shallow donor, but incorporation of La on the Sn site can lead to self-compensation. At low La concentrations and in O-poor conditions, oxygen vacancies form in BaSnO3. A-site cation vacancies are found to be dominant among the native compensating centers. Compared to BaSnO3, charge compensation is a larger problem for the wider-band-gap stannates, SrSnO3 and CaSnO3, a trend we can explain based on conduction-band alignments. The formation of compensating acceptor defects can be inhibited by choosing oxygen-poor (cation-rich) growth or annealing conditions, thus providing a pathway for improved n-type doping.

The experimental determination of valence band offsets (VBOs) at interfaces in complex-oxide heterostructures using conventional soft x-ray photoelectron spectroscopy (SXPS, h 1500 eV) and reference core-level binding energies can present challenges because of surface charging when photoelectrons are emitted and insufficient probing depth to clearly resolve the interfaces. In this paper, we compare VBOs measured with SXPS and its multi-keV hard x-ray analogue (HXPS, h > 2000 eV). We demonstrate that the use of HXPS allows one to minimize charging effects and to probe more deeply buried interfaces in heterostructures such as SrTiO 3 /LaNiO 3 and SrTiO 3 / GdTiO 3. The VBO values obtained by HXPS for these interfaces are furthermore found to be close to those determined by first-principles calculations. V