Tailoring a two-dimensional electron gas at the LaAlO3/SrTiO3 (001) interface by epitaxial strain

Recently a metallic state was discovered at the interface between insulating oxides, most notably LaAlO3 and SrTiO3. Properties of this two-dimensional electron gas (2DEG) have attracted significant interest due to its potential applications in nanoelectronics. Control over this carrier density and mobility of the 2DEG is essential for applications of these novel systems, and may be achieved by epitaxial strain. However, despite the rich nature of strain effects on oxide materials properties, such as ferroelectricity, magnetism, and superconductivity, the relationship between the strain and electrical properties of the 2DEG at the LaAlO3/SrTiO3 heterointerface remains largely unexplored. Here, we use different lattice constant single crystal substrates to produce LaAlO3/SrTiO3 interfaces with controlled levels of biaxial epitaxial strain. We have found that tensile strained SrTiO3 destroys the conducting 2DEG, while compressively strained SrTiO3 retains the 2DEG, but with a carrier concentration reduced in comparison to the unstrained LaAlO3/SrTiO3 interface. We have also found that the critical LaAlO3 overlayer thickness for 2DEG formation increases with SrTiO3 compressive strain. Our first-principles calculations suggest that a strain-induced electric polarization in the SrTiO3 layer is responsible for this behavior. It is directed away from the interface and hence creates a negative polarization charge opposing that of the polar LaAlO3 layer. This both increases the critical thickness of the LaAlO3 layer, and reduces carrier concentration above the critical thickness, in agreement with our experimental results. Our findings suggest that epitaxial strain can be used to tailor 2DEGs properties of the LaAlO3/SrTiO3 heterointerface

Structural and Electronic Properties of the Interface between the High-k oxide LaAlO3 and Si(001)

The structural and electronic properties of the LaAlO3/Si(001) interface are determined using state-of-the-art electronic structure calculations. The atomic structure differs from previous proposals, but is reminiscent of La adsorption structures on silicon. A phase diagram of the interface stability is calculated as a function of oxygen and Al chemical potentials. We find that an electronically saturated interface is obtained only if dopant atoms segregate to the interface. These findings raise serious doubts whether LaAlO3 can be used as an epitaxial gate dielectric.Comment: 4 pages, 5 figure

High-Resolution Crystal Truncation Rod Scattering: Application to Ultrathin Layers and Buried Interfaces

In crystalline materials, the presence of surfaces or interfaces gives rise to crystal truncation rods (CTRs) in their X‐ray diffraction patterns. While structural properties related to the bulk of a crystal are contained in the intensity and position of Bragg peaks in X‐ray diffraction, CTRs carry detailed information about the atomic structure at the interface. Developments in synchrotron X‐ray sources, instrumentation, and analysis procedures have made CTR measurements into extremely powerful tools to study atomic reconstructions and relaxations occurring in a wide variety of interfacial systems, with relevance to chemical and electronic functionalities. In this review, an overview of the use of CTRs in the study of atomic structure at interfaces is provided. The basic theory, measurement, and analysis of CTRs are covered and applications from the literature are highlighted. Illustrative examples include studies of complex oxide thin films and multilayers

Long-range electronic reconstruction to a dxz,yzd_{xz,yz}-dominated Fermi surface below the LaAlO3_3/SrTiO3_3 interface

Low dimensionality, broken symmetry and easily-modulated carrier concentrations provoke novel electronic phase emergence at oxide interfaces. However, the spatial extent of such reconstructions - i.e. the interfacial "depth" - remains unclear. Examining LaAlO$_3$/SrTiO$_3$ heterostructures at previously unexplored carrier densities $n_{2D}\geq6.9\times10^{14}$ cm$^{-2}$, we observe a Shubnikov-de Haas effect for small in-plane fields, characteristic of an anisotropic 3D Fermi surface with preferential $d_{xz,yz}$ orbital occupancy extending over at least 100~nm perpendicular to the interface. Quantum oscillations from the 3D Fermi surface of bulk doped SrTiO$_3$ emerge simultaneously at higher $n_{2D}$. We distinguish three areas in doped perovskite heterostructures: narrow ($<20$ nm) 2D interfaces housing superconductivity and/or other emergent phases, electronically isotropic regions far ($>120$ nm) from the interface and new intermediate zones where interfacial proximity renormalises the electronic structure relative to the bulk.Comment: Supplementary material available at Scientific Reports websit

Formation and observation of a quasi-two-dimensional dxyd_{xy} electron liquid in epitaxially stabilized Sr2−x_{2-x}Lax_{x}TiO4_{4} thin films

We report the formation and observation of an electron liquid in Sr$_{2-x}$La$_{x}$TiO$_4$, the quasi-two-dimensional counterpart of SrTiO$_3$, through reactive molecular-beam epitaxy and {\it in situ} angle-resolved photoemission spectroscopy. The lowest lying states are found to be comprised of Ti 3$d_{xy}$ orbitals, analogous to the LaAlO$_3$/SrTiO$_3$ interface and exhibit unusually broad features characterized by quantized energy levels and a reduced Luttinger volume. Using model calculations, we explain these characteristics through an interplay of disorder and electron-phonon coupling acting co-operatively at similar energy scales, which provides a possible mechanism for explaining the low free carrier concentrations observed at various oxide heterostructures such as the LaAlO$_3$/SrTiO$_3$ interface

Atomically flat interface between a single-terminated LaAlO3 substrate and SrTiO3 thin film is insulating

The surface termination of (100)-oriented LaAlO3 (LAO) single crystals was examined by atomic force microscopy and optimized to produce a single-terminated atomically flat surface by annealing. Then the atomically flat STO film was achieved on a single-terminated LAO substrate, which is expected to be similar to the n-type interface of two-dimensional electron gas (2DEG), i.e., (LaO)-(TiO2). Particularly, that can serve as a mirror structure for the typical 2DEG heterostructure to further clarify the origin of 2DEG. This newly developed interface was determined to be highly insulating. Additionally, this study demonstrates an approach to achieve atomically flat film growth based on LAO substrates.Comment: 4 pages, 3 figure