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Register a new userNon-collinear and strongly asymmetric polar moments at back-gated SrTiO3 interfaces
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The highly mobile electrons at the interface of SrTiO3 with other oxide insulators, such as LaAlO3 or AlOx, are of great current interest. A vertical gate voltage allows controlling a metal/superconductor-to-insulator transition, as well as electrical modulation of the spin-orbit Rashba coupling for spin-charge conversion. These findings raise important questions about the origin of the confined electrons as well as the mechanisms that govern the interfacial electric field. Here we use infrared ellipsometry and confocal Raman spectroscopy to show that an anomalous polar moment is induced at the interface that is non-collinear, highly asymmetric and hysteretic with respect to the vertical gate electric field. Our data indicate that an important role is played by the electromigration of oxygen vacancies and their clustering at the antiferrodistortive domain boundaries of SrTiO3, which generates local electric and possibly also flexoelectric fields and subsequent polar moments with a large lateral component. Our results open new perspectives for the defect engineering of lateral devices with strongly enhanced and hysteretic local electric fields that can be manipulated with various other parameters, like strain, temperature, or photons.
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In recent years, striking discoveries have revealed that two-dimensional electron liquids (2DEL) confined at the interface between oxide band-insulators can be engineered to display a high mobility transport. The recognition that only few interfaces appear to suit hosting 2DEL is intriguing and challenges the understanding of these emerging properties not existing in bulk. Indeed, only the neutral TiO2 surface of (001)SrTiO3 has been shown to sustain 2DEL. We show that this restriction can be surpassed: (110) and (111) surfaces of SrTiO3 interfaced with epitaxial LaAlO3 layers, above a critical thickness, display 2DEL transport with mobilities similar to those of (001)SrTiO3. Moreover we show that epitaxial interfaces are not a prerequisite: conducting (110) interfaces with amorphous LaAlO3 and other oxides can also be prepared. These findings open a new perspective both for materials research and for elucidating the ultimate microscopic mechanism of carrier doping.
The interfacial screening charge that arises to compensate electric fields of dielectric or ferroelectric thin films is now recognized as the most important factor in determining the capacitance or polarization of ultrathin ferroelectrics. Here we investigate using aberration-corrected electron microscopy and density functional theory how interfaces cope with the need to terminate ferroelectric polarization. In one case, we show evidence for ionic screening, which has been predicted by theory but never observed. For a ferroelectric film on an insulating substrate, we found that compensation can be mediated by interfacial charge generated, for example, by oxygen vacancies.
Control of order-disorder phase transitions is a fundamental materials science challenge, underpinning the development of energy storage technologies such as solid oxide fuel cells and batteries, ultra-high temperature ceramics, and durable nuclear waste forms. At present, the development of promising complex oxides for these applications is hindered by a poor understanding of how interfaces affect lattice disordering processes and defect transport. Here we explore the evolution of local disorder in ion-irradiated La$_2$Ti$_2$O$_7$ / SrTiO$_3$ thin film heterostructures using a combination of high-resolution scanning transmission electron microscopy (STEM), position-averaged convergent beam electron diffraction (PACBED), electron energy loss spectroscopy (STEM-EELS), and textit{ab initio} theory calculations. We observe highly non-uniform lattice disordering driven by asymmetric oxygen vacancy formation across the interface. Our calculations indicate that this asymmetry results from differences in the polyhedral connectivity and vacancy formation energies of the two interface components, suggesting ways to manipulate lattice disorder in functional oxide heterostructures.
Using a low-temperature conductive-tip atomic force microscope in cross-section geometry we have characterized the local transport properties of the metallic electron gas that forms at the interface between LaAlO3 and SrTiO3. At low temperature, we find that the carriers do not spread away from the interface but are confined within ~10 nm, just like at room temperature. Simulations taking into account both the large temperature and electric-field dependence of the permittivity of SrTiO3 predict a confinement over a few nm for sheet carrier densities larger than ~6 10^13 cm-2. We discuss the experimental and simulations results in terms of a multi-band carrier system. Remarkably, the Fermi wavelength estimated from Hall measurements is ~16 nm, indicating that the electron gas in on the verge of two-dimensionality.
Using tunneling spectroscopy we have measured the spectral density of states of the mobile, two-dimensional electron system generated at the LaAlO3-SrTiO3 interface. As shown by the density of states the interface electron system differs qualitatively, first, from the electron systems of the materials defining the interface and, second, from the two-dimensional electron gases formed at interfaces between conventional semiconductors.
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