Tuning Oxide Properties by Oxygen Vacancy Control During Growth and Annealing.

Electrical, optical, and magnetic properties of oxide materials can often be controlled by varying the oxygen content. Here we outline two approaches for varying the oxygen content and provide concrete examples for tuning the electrical properties of SrTiO3-based heterostructures. In the first approach, the oxygen content is controlled by varying the deposition parameters during a pulsed laser deposition. In the second approach, the oxygen content is tuned by subjecting the samples to annealing in oxygen at elevated temperatures after the film growth. The approaches can be used for a wide range of oxides and nonoxide materials where the properties are sensitive to a change in the oxidation state. The approaches differ significantly from electrostatic gating, which is often used to change the electronic properties of confined electronic systems such as those observed in SrTiO3-based heterostructures. By controlling the oxygen vacancy concentration, we are able to control the carrier density over many orders of magnitude, even in nonconfined electronic systems. Moreover, properties can be controlled, which are not sensitive to the density of itinerant electrons.

Controlled Electronic and Magnetic Landscape in Self-Assembled Complex Oxide Heterostructures.

Complex oxide heterointerfaces contain a rich playground of novel physical properties and functionalities, which give rise to emerging technologies. Among designing and controlling the functional properties of complex oxide film heterostructures, vertically aligned nanostructure (VAN) films using a self-assembling bottom-up deposition method presents great promise in terms of structural flexibility and property tunability. Here, the bottom-up self-assembly is extended to a new approach using a mixture containing a 2Dlayer-by-layer film growth, followed by a 3D VAN film growth. In this work, the two-phase nanocomposite thin films are based on LaAlO3 :LaBO3 , grown on a lattice-mismatched SrTiO3001 (001) single crystal. The 2D-to-3D transient structural assembly is primarily controlled by the composition ratio, leading to the coexistence of multiple interfacial properties, 2D electron gas, and magnetic anisotropy. This approach provides multidimensional film heterostructures which enrich the emergent phenomena for multifunctional applications.

Stacking and Twisting of Freestanding Complex Oxide Thin Films.

The integration of dissimilar materials in heterostructures has long been a cornerstone of modern materials science-seminal examples are 2D materials and van der Waals heterostructures. Recently, new methods have been developed that enable the realization of ultrathin freestanding oxide films approaching the 2D limit. Oxides offer new degrees of freedom, due to the strong electronic interactions, especially the 3d orbital electrons, which give rise to rich exotic phases. Inspired by this progress, a new platform for assembling freestanding oxide thin films with different materials and orientations into artificial stacks with heterointerfaces is developed. It is shown that the oxide stacks can be tailored by controlling the stacking sequences, as well as the twist angle between the constituent layers with atomically sharp interfaces, leading to distinct moiré patterns in the transmission electron microscopy images of the full stacks. Stacking and twisting is recognized as a key degree of structural freedom in 2D materials but, until now, has never been realized for oxide materials. This approach opens unexplored avenues for fabricating artificial 3D oxide stacking heterostructures with freestanding membranes across a broad range of complex oxide crystal structures with functionalities not available in conventional 2D materials.

A Two-Dimensional Superconducting Electron Gas in Freestanding LaAlO3/SrTiO3 Micromembranes.

Freestanding oxide membranes constitute an intriguing material platform for new functionalities and allow integration of oxide electronics with technologically important platforms such as silicon. Sambri et al. recently reported a method to fabricate freestanding LaAlO3/SrTiO3 (LAO/STO) membranes by spalling of strained heterostructures. Here, we first develop a scheme for the high-yield fabrication of membrane devices on silicon. Second, we show that the membranes exhibit metallic conductivity and a superconducting phase below ∼200 mK. Using anisotropic magnetotransport we extract the superconducting phase coherence length ξ ≈ 36-80 nm and establish an upper bound on the thickness of the superconducting electron gas d ≈ 17-33 nm, thus confirming its two-dimensional character. Finally, we show that the critical current can be modulated using a silicon-based backgate. The ability to form superconducting nanostructures of LAO/STO membranes, with electronic properties similar to those of the bulk counterpart, opens opportunities for integrating oxide nanoelectronics with silicon-based architectures.

Ultrahigh Carrier Mobilities in Ferroelectric Domain Wall Corbino Cones at Room Temperature.

Recently, electrically conducting heterointerfaces between dissimilar band insulators (such as lanthanum aluminate and strontium titanate) have attracted considerable research interest. Charge transport and fundamental aspects of conduction have been thoroughly explored. Perhaps surprisingly, similar studies on conceptually much simpler conducting homointerfaces, such as domain walls, are not nearly so well developed. Addressing this disparity, magnetoresistance is herein reported in approximately conical 180° charged domain walls, in partially switched ferroelectric thin-film single-crystal lithium niobate. This system is ideal for such measurements: first, the conductivity difference between domains and domain walls is unusually large (a factor of 1013 ) and hence currents driven through the thin film, between planar top and bottom electrodes, are overwhelmingly channeled along the walls; second, when electrical contact is made to the top and bottom of the domain walls and a magnetic field is applied along their cone axes, then the test geometry mirrors that of a Corbino disk: a textbook arrangement for geometric magnetoresistance measurement. Data imply carriers with extremely high room-temperature Hall mobilities of up to ≈3700 cm2 V-1 s-1 . This is an unparalleled value for oxide interfaces (and for bulk oxides) comparable to mobilities in other systems seen at cryogenic, rather than at room, temperature.

Nonreciprocal Transport in a Rashba Ferromagnet, Delafossite PdCoO2.

Rashba interfaces yield efficient spin-charge interconversion and give rise to nonreciprocal transport phenomena. Here, we report magnetotransport experiments in few-nanometer-thick films of PdCoO2, a delafossite oxide known to display a large Rashba splitting and surface ferromagnetism. By analyzing the angle dependence of the first- and second-harmonic longitudinal and transverse resistivities, we identify a Rashba-driven unidirectional magnetoresistance that competes with the anomalous Nernst effect below the Curie point. We estimate a Rashba coefficient of 0.75 ± 0.3 eV Å and argue that our results qualify delafossites as a new family of oxides for nanospintronics and spin-orbitronics, beyond perovskite materials.

Spin-Charge Interconversion in KTaO3 2D Electron Gases.

Oxide interfaces exhibit a broad range of physical effects stemming from broken inversion symmetry. In particular, they can display non-reciprocal phenomena when time reversal symmetry is also broken, e.g., by the application of a magnetic field. Examples include the direct and inverse Edelstein effects (DEE, IEE) that allow the interconversion between spin currents and charge currents. The DEE and IEE have been investigated in interfaces based on the perovskite SrTiO3 (STO), albeit in separate studies focusing on one or the other. The demonstration of these effects remains mostly elusive in other oxide interface systems despite their blossoming in the last decade. Here, the observation of both the DEE and IEE in a new interfacial two-dimensional electron gas (2DEG) based on the perovskite oxide KTaO3 is reported. 2DEGs are generated by the simple deposition of Al metal onto KTaO3 single crystals, characterized by angle-resolved photoemission spectroscopy and magnetotransport, and shown to display the DEE through unidirectional magnetoresistance and the IEE by spin-pumping experiments. Their spin-charge interconversion efficiency is then compared with that of STO-based interfaces, related to the 2DEG electronic structure, and perspectives are given for the implementation of KTaO3 2DEGs into spin-orbitronic devices is compared.

Size-Controlled Spalling of LaAlO3/SrTiO3 Micromembranes.

The ability to form freestanding oxide membranes of nanoscale thickness is of great interest for enabling material functionality and for integrating oxides in flexible electronic and photonic technologies. Recently, a route has been demonstrated for forming conducting heterostructure membranes of LaAlO3 and SrTiO3, the canonical system for oxide electronics. In this route, the epitaxial growth of LaAlO3 on SrTiO3 resulted in a strained state that relaxed by producing freestanding membranes with random sizes and locations. Here, we extend the method to enable self-formed LaAlO3/SrTiO3 micromembranes with control over membrane position, their lateral sizes from 2 to 20 µm, and with controlled transfer to other substrates of choice. This method opens up the possibility to study and use the two-dimensional electron gas in LaAlO3/SrTiO3 membranes for advanced device concepts.

Non-volatile electric control of spin-charge conversion in a SrTiO3 Rashba system.

After 50 years of development, the technology of today's electronics is approaching its physical limits, with feature sizes smaller than 10 nanometres. It is also becoming clear that the ever-increasing power consumption of information and communication systems1 needs to be contained. These two factors require the introduction of non-traditional materials and state variables. As recently highlighted2, the remanence associated with collective switching in ferroic systems is an appealing way to reduce power consumption. A promising approach is spintronics, which relies on ferromagnets to provide non-volatility and to generate and detect spin currents3. However, magnetization reversal by spin transfer torques4 is a power-consuming process. This is driving research on multiferroics to achieve low-power electric-field control of magnetization5, but practical materials are scarce and magnetoelectric switching remains difficult to control. Here we demonstrate an alternative strategy to achieve low-power spin detection, in a non-magnetic system. We harness the electric-field-induced ferroelectric-like state of strontium titanate (SrTiO3)6-9 to manipulate the spin-orbit properties10 of a two-dimensional electron gas11, and efficiently convert spin currents into positive or negative charge currents, depending on the polarization direction. This non-volatile effect opens the way to the electric-field control of spin currents and to ultralow-power spintronics, in which non-volatility would be provided by ferroelectricity rather than by ferromagnetism.

Electric-Field Control of Spin Current Generation and Detection in Ferromagnet-Free SrTiO3-Based Nanodevices.

Spintronics entails the generation, transport, manipulation and detection of spin currents, usually in hybrid architectures comprising interfaces whose impact on performance is detrimental. In addition, how spins are generated and detected is generally material specific and determined by the electronic structure. Here, we demonstrate spin current generation, transport and electrical detection, all within a single non-magnetic material system: a SrTiO3 two-dimensional electron gas (2DEG) with Rashba spin-orbit coupling. We show that the spin current is generated from a charge current by the 2D spin Hall effect, transported through a channel and reconverted into a charge current by the inverse 2D spin Hall effect. Furthermore, by adjusting the Fermi energy with a gate voltage we tune the generated and detected spin polarization and relate it to the complex multiorbital band structure of the 2DEG. We discuss the leading mechanisms of the spin-charge interconversion processes and argue for the potential of quantum oxide materials for future all-electrical low-power spin-based logic.

Imaging and Harnessing Percolation at the Metal-Insulator Transition of NdNiO3 Nanogaps.

Competition between coexisting electronic phases in first-order phase transitions can lead to a sharp change in the resistivity as the material is subjected to small variations in the driving parameter, for example, the temperature. One example of this phenomenon is the metal-insulator transition (MIT) in perovskite rare-earth nickelates. In such systems, reducing the transport measurement area to dimensions comparable to the domain size of insulating and metallic phases around the MIT should strongly influence the shape of the resistance-temperature curve. Here we measure the temperature dependence of the local resistance and the nanoscale domain distribution of NdNiO3 areas between Au contacts gapped by 40-260 nm. We find that a sharp resistance drop appears below the bulk MIT temperature at ∼105 K, with an amplitude inversely scaling with the nanogap width. By using X-ray photoemission electron microscopy, we directly correlate the resistance drop to the emergence and distribution of individual metallic domains at the nanogap. Our observation provides useful insight into percolation at the MIT of rare-earth nickelates.

Mapping spin-charge conversion to the band structure in a topological oxide two-dimensional electron gas.

While spintronics has traditionally relied on ferromagnetic metals as spin generators and detectors, spin-orbitronics exploits the efficient spin-charge interconversion enabled by spin-orbit coupling in non-magnetic systems. Although the Rashba picture of split parabolic bands is often used to interpret such experiments, it fails to explain the largest conversion effects and their relationship with the electronic structure. Here, we demonstrate a very large spin-to-charge conversion effect in an interface-engineered, high-carrier-density SrTiO3 two-dimensional electron gas and map its gate dependence on the band structure. We show that the conversion process is amplified by enhanced Rashba-like splitting due to orbital mixing and in the vicinity of avoided band crossings with topologically non-trivial order. Our results indicate that oxide two-dimensional electron gases are strong candidates for spin-based information readout in new memory and transistor designs. Our results also emphasize the promise of topology as a new ingredient to expand the scope of complex oxides for spintronics.

Direct Mapping of Phase Separation across the Metal-Insulator Transition of NdNiO3.

Perovskite rare-earth nickelates RNiO3 are prototype correlated oxides displaying a metal-insulator transition (MIT) at a temperature tunable by the ionic radius of the rare-earth R. Although its precise origin remains a debated topic, the MIT can be exploited in various types of applications, notably for resistive switching and neuromorphic computation. So far, the MIT has been mostly studied by macroscopic techniques, and insights into its nanoscale mechanisms were only provided recently by X-ray photoemission electron microscopy through absorption line shifts, used as an indirect proxy to the resistive state. Here, we directly image the local resistance of NdNiO3 thin films across their first-order MIT using conductive-atomic force microscopy. Our resistance maps reveal the nucleation of ∼100-300 nm metallic domains in the insulating state that grow and percolate as temperature increases. We discuss the resistance contrast mechanism, analyze the microscopy and transport data within a percolation model, and propose experiments to harness this mesoscopic electronic texture in devices.

Transport and excitations in a negative-U quantum dot at the LaAlO3/SrTiO3 interface.

In a solid-state host, attractive electron-electron interactions can lead to the formation of local electron pairs which play an important role in the understanding of prominent phenomena such as high T c superconductivity and the pseudogap phase. Recently, evidence of a paired ground state without superconductivity was demonstrated at the level of single electrons in quantum dots at the interface of LaAlO3 and SrTiO3. Here, we present a detailed study of the excitation spectrum and transport processes of a gate-defined LaAlO3/SrTiO3 quantum dot exhibiting pairing at low temperatures. For weak tunneling, the spectrum agrees with calculations based on the Anderson model with a negative effective charging energy U, and exhibits an energy gap corresponding to the Zeeman energy of the magnetic pair-breaking field. In contrast, for strong coupling, low-bias conductance is enhanced with a characteristic dependence on temperature, magnetic field and chemical potential consistent with the charge Kondo effect.Complex oxide devices provide a platform for studying and making use of strongly correlated electronic behavior. Here the authors present a LaAlO3/SrTiO3 quantum dot and show that its transport behavior is consistent with the presence of attractive electron interactions and the charge Kondo effect.

Quantization of Hall Resistance at the Metallic Interface between an Oxide Insulator and SrTiO_{3}.

The two-dimensional metal forming at the interface between an oxide insulator and SrTiO_{3} provides new opportunities for oxide electronics. However, the quantum Hall effect, one of the most fascinating effects of electrons confined in two dimensions, remains underexplored at these complex oxide heterointerfaces. Here, we report the experimental observation of quantized Hall resistance in a SrTiO_{3} heterointerface based on the modulation-doped amorphous-LaAlO_{3}/SrTiO_{3} heterostructure, which exhibits both high electron mobility exceeding 10,000 cm^{2}/V s and low carrier density on the order of ∼10^{12} cm^{-2}. Along with unambiguous Shubnikov-de Haas oscillations, the spacing of the quantized Hall resistance suggests that the interface is comprised of a single quantum well with ten parallel conducting two-dimensional sub-bands. This provides new insight into the electronic structure of conducting oxide interfaces and represents an important step towards designing and understanding advanced oxide devices.

Creation of high mobility two-dimensional electron gases via strain induced polarization at an otherwise nonpolar complex oxide interface.

The discovery of two-dimensional electron gases (2DEGs) in SrTiO3-based heterostructures provides new opportunities for nanoelectronics. Herein, we create a new type of oxide 2DEG by the epitaxial-strain-induced polarization at an otherwise nonpolar perovskite-type interface of CaZrO3/SrTiO3. Remarkably, this heterointerface is atomically sharp and exhibits a high electron mobility exceeding 60,000 cm(2) V(-1) s(-1) at low temperatures. The 2DEG carrier density exhibits a critical dependence on the film thickness, in good agreement with the polarization induced 2DEG scheme.