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Register a new userCoupling charge and topological reconstructions at polar oxide interfaces
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In oxide heterostructures, different materials are integrated into a single artificial crystal, resulting in a breaking of inversion-symmetry across the heterointerfaces. A notable example is the interface between polar and non-polar materials, where valence discontinuities lead to otherwise inaccessible charge and spin states. This approach paved the way to the discovery of numerous unconventional properties absent in the bulk constituents. However, control of the geometric structure of the electronic wavefunctions in correlated oxides remains an open challenge. Here, we create heterostructures consisting of ultrathin SrRuO$_3$, an itinerant ferromagnet hosting momentum-space sources of Berry curvature, and LaAlO$_3$, a polar wide-bandgap insulator. Transmission electron microscopy reveals an atomically sharp LaO/RuO$_2$/SrO interface configuration, leading to excess charge being pinned near the LaAlO$_3$/SrRuO$_3$ interface. We demonstrate through magneto-optical characterization, theoretical calculations and transport measurements that the real-space charge reconstruction modifies the momentum-space Berry curvature in SrRuO$_3$, driving a reorganization of the topological charges in the band structure. Our results illustrate how the topological and magnetic features of oxides can be manipulated by engineering charge discontinuities at oxide interfaces.
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The interface between the insulators LaAlO$_3$ and SrTiO$_3$ accommodates a two-dimensional electron liquid (2DEL) -- a high mobility electron system exhibiting superconductivity as well as indications of magnetism and correlations. While this flagship oxide heterostructure shows promise for electronics applications, the origin and microscopic properties of the 2DEL remain unclear. The uncertainty remains in part because the electronic structures of such nanoscale buried interfaces are difficult to probe, and is compounded by the variable presence of oxygen vacancies and coexistence of both localized and delocalized charges. These various complications have precluded decisive tests of intrinsic electronic and orbital reconstruction at this interface. Here we overcome prior difficulties by developing an interface analysis based on the inherently interface-sensitive resonant x-ray reflectometry. We discover a high charge density of 0.5 electrons per interfacial unit cell for samples above the critical LaAlO$_3$ thickness, and extract the depth dependence of both the orbital and electronic reconstructions near the buried interface. We find that the majority of the reconstruction phenomena are confined to within 2 unit cells of the interface, and we quantify how oxygen vacancies significantly affect the electronic system. Our results provide strong support for the existence of polarity induced electronic reconstruction, clearly separating its effects from those of oxygen vacancies.
Since the discovery of two-dimensional electron gas (2DEG) at the oxide interface of LaAlO3/SrTiO3, improving carrier mobility has become an important issue for device applications. In this paper, by using an alternate polar perovskite insulator (La0.3Sr0.7)(Al0.65Ta0.35)O3 (LSAT) for reducing lattice mismatch from 3.0% to 1.0%, the low-temperature carrier mobility has been increased 30 fold to 35,000 cm2V-1s-1. Moreover, two critical thicknesses for the LSAT/SrTiO3 (001) interface are found: one at 5 unit cell for appearance of the 2DEG, the other at 12 unit cell for a peak in the carrier mobility. By contrast, the conducting (110) and (111) LSAT/STO interfaces only show a single critical thickness of 8 unit cells. This can be explained in terms of polar fluctuation arising from LSAT chemical composition. In addition to lattice mismatch and crystal symmetry at the interface, polar fluctuation arising from composition has been identified as an important variable to be tailored at the oxide interfaces to optimise the 2DEG transport.
Atomically sharp oxide heterostructures exhibit a range of novel physical phenomena that do not occur in the parent bulk compounds. The most prominent example is the appearance of highly conducting and superconducting states at the interface between the band insulators LaAlO3 and SrTiO3. Here we report a new emergent phenomenon at the LaMnO3/SrTiO3 interface in which an antiferromagnetic insulator abruptly transforms into a magnetic state that exhibits unexpected nanoscale superparamagnetic dynamics. Upon increasing the thickness of LaMnO3 above five unit cells, our scanning nanoSQUID-on-tip microscopy shows spontaneous formation of isolated magnetic islands of 10 to 50 nm diameter, which display random moment reversals by thermal activation or in response to an in-plane magnetic field. Our charge reconstruction model of the polar LaMnO3/SrTiO3 heterostructure describes the sharp emergence of thermodynamic phase separation leading to nucleation of metallic ferromagnetic islands in an insulating antiferromagnetic matrix. The model further suggests that the nearby superparamagnetic-ferromagnetic transition can be gate tuned, holding potential for applications in magnetic storage and spintronics.
The discovery of two-dimensional electron gases (2DEGs) at the interface between two insulating complex oxides, such as LaAlO3 (LAO) or gamma-Al2O3 (GAO) epitaxially grown on SrTiO3 (STO) 1,2, provides an opportunity for developing all-oxide electronic devices3,4. These 2DEGs at complex oxide interfaces involve many-body interactions and give rise to a rich set of phenomena5, for example, superconductivity6, magnetism7,8, tunable metal-insulator transitions9, and phase separation10. However, large enhancement of the interfacial electron mobility remains a major and long-standing challenge for fundamental as well as applied research of complex oxides11-15. Here, we inserted a single unit cell insulating layer of polar La1-xSrxMnO3 (x=0, 1/8, and 1/3) at the interface between disordered LaAlO3 and crystalline SrTiO3 created at room temperature. We find that the electron mobility of the interfacial 2DEG is enhanced by more than two orders of magnitude. Our in-situ and resonant x-ray spectroscopic in addition to transmission electron microscopy results indicate that the manganite layer undergoes unambiguous electronic reconstruction and leads to modulation doping of such atomically engineered complex oxide heterointerfaces. At low temperatures, the modulation-doped 2DEG exhibits clear Shubnikov-de Haas oscillations and the initial manifestation of the quantum Hall effect, demonstrating an unprecedented high-mobility and low electron density oxide 2DEG system. These findings open new avenues for oxide electronics.
By means of a Wannier projection within the framework of density functional theory, we are able to identify the modified c-axis hopping and the energy mismatch between the cation bands as the main source of the $t_{2g}$ splitting around the $Gamma$ point for oxide heterostructures, excluding previously proposed mechanisms such as Jahn-Teller distortions or electric field asymmetries. Interfacing LaAlO$_3$, LaVO$_3$, SrVO$_3$ and SrNbO$_3$ with SrTiO$_3$ we show how to tune this orbital splitting, designing heterostructures with more $d_{xy}$ electrons at the interface. Such an orbital engineering is the key for controlling the physical properties at the interface of oxide heterostructures.
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