In-plane quasi-single-domain BaTiO3 via interfacial symmetry engineering.

The control of the in-plane domain evolution in ferroelectric thin films is not only critical to understanding ferroelectric phenomena but also to enabling functional device fabrication. However, in-plane polarized ferroelectric thin films typically exhibit complicated multi-domain states, not desirable for optoelectronic device performance. Here we report a strategy combining interfacial symmetry engineering and anisotropic strain to design single-domain, in-plane polarized ferroelectric BaTiO3 thin films. Theoretical calculations predict the key role of the BaTiO3/PrScO3 [Formula: see text] substrate interfacial environment, where anisotropic strain, monoclinic distortions, and interfacial electrostatic potential stabilize a single-variant spontaneous polarization. A combination of scanning transmission electron microscopy, piezoresponse force microscopy, ferroelectric hysteresis loop measurements, and second harmonic generation measurements directly reveals the stabilization of the in-plane quasi-single-domain polarization state. This work offers design principles for engineering in-plane domains of ferroelectric oxide thin films, which is a prerequisite for high performance optoelectronic devices.

Controlling spin current polarization through non-collinear antiferromagnetism.

The interconversion of charge and spin currents via spin-Hall effect is essential for spintronics. Energy-efficient and deterministic switching of magnetization can be achieved when spin polarizations of these spin currents are collinear with the magnetization. However, symmetry conditions generally restrict spin polarizations to be orthogonal to both the charge and spin flows. Spin polarizations can deviate from such direction in nonmagnetic materials only when the crystalline symmetry is reduced. Here, we show control of the spin polarization direction by using a non-collinear antiferromagnet Mn3GaN, in which the triangular spin structure creates a low magnetic symmetry while maintaining a high crystalline symmetry. We demonstrate that epitaxial Mn3GaN/permalloy heterostructures can generate unconventional spin-orbit torques at room temperature corresponding to out-of-plane and Dresselhaus-like spin polarizations which are forbidden in any sample with two-fold rotational symmetry. Our results demonstrate an approach based on spin-structure design for controlling spin-orbit torque, enabling high-efficient antiferromagnetic spintronics.

Anisotropic spin-orbit torque generation in epitaxial SrIrO3 by symmetry design.

Spin-orbit coupling (SOC), the interaction between the electron spin and the orbital angular momentum, can unlock rich phenomena at interfaces, in particular interconverting spin and charge currents. Conventional heavy metals have been extensively explored due to their strong SOC of conduction electrons. However, spin-orbit effects in classes of materials such as epitaxial 5d-electron transition-metal complex oxides, which also host strong SOC, remain largely unreported. In addition to strong SOC, these complex oxides can also provide the additional tuning knob of epitaxy to control the electronic structure and the engineering of spin-to-charge conversion by crystalline symmetry. Here, we demonstrate room-temperature generation of spin-orbit torque on a ferromagnet with extremely high efficiency via the spin-Hall effect in epitaxial metastable perovskite SrIrO3 We first predict a large intrinsic spin-Hall conductivity in orthorhombic bulk SrIrO3 arising from the Berry curvature in the electronic band structure. By manipulating the intricate interplay between SOC and crystalline symmetry, we control the spin-Hall torque ratio by engineering the tilt of the corner-sharing oxygen octahedra in perovskite SrIrO3 through epitaxial strain. This allows the presence of an anisotropic spin-Hall effect due to a characteristic structural anisotropy in SrIrO3 with orthorhombic symmetry. Our experimental findings demonstrate the heteroepitaxial symmetry design approach to engineer spin-orbit effects. We therefore anticipate that these epitaxial 5d transition-metal oxide thin films can be an ideal building block for low-power spintronics.

Isostructural metal-insulator transition in VO2.

The metal-insulator transition in correlated materials is usually coupled to a symmetry-lowering structural phase transition. This coupling not only complicates the understanding of the basic mechanism of this phenomenon but also limits the speed and endurance of prospective electronic devices. We demonstrate an isostructural, purely electronically driven metal-insulator transition in epitaxial heterostructures of an archetypal correlated material, vanadium dioxide. A combination of thin-film synthesis, structural and electrical characterizations, and theoretical modeling reveals that an interface interaction suppresses the electronic correlations without changing the crystal structure in this otherwise correlated insulator. This interaction stabilizes a nonequilibrium metallic phase and leads to an isostructural metal-insulator transition. This discovery will provide insights into phase transitions of correlated materials and may aid the design of device functionalities.

Direct observation of room-temperature out-of-plane ferroelectricity and tunneling electroresistance at the two-dimensional limit.

Out-of-plane ferroelectricity with a high transition temperature in nanometer-scale films is required to miniaturize electronic devices. Direct visualization of stable ferroelectric polarization and its switching behavior in atomically thick films is critical for achieving this goal. Here, ferroelectric order at room temperature in the two-dimensional limit is demonstrated in tetragonal BiFeO3 ultrathin films. Using aberration-corrected scanning transmission electron microscopy, we directly observed robust out-of-plane spontaneous polarization in one-unit-cell-thick BiFeO3 films. High-resolution piezoresponse force microscopy measurements show that the polarization is stable and switchable, whereas a tunneling electroresistance effect of up to 370% is achieved in BiFeO3 films. Based on first-principles calculations and Kelvin probe force microscopy measurements, we explain the mechanism of polarization stabilization by the ionic displacements in oxide electrode and the surface charges. Our results indicate that critical thickness for ferroelectricity in the BiFeO3 film is virtually absent, making it a promising candidate for high-density nonvolatile memories.

Ambipolar ferromagnetism by electrostatic doping of a manganite.

Complex-oxide materials exhibit physical properties that involve the interplay of charge and spin degrees of freedom. However, an ambipolar oxide that is able to exhibit both electron-doped and hole-doped ferromagnetism in the same material has proved elusive. Here we report ambipolar ferromagnetism in LaMnO3, with electron-hole asymmetry of the ferromagnetic order. Starting from an undoped atomically thin LaMnO3 film, we electrostatically dope the material with electrons or holes according to the polarity of a voltage applied across an ionic liquid gate. Magnetotransport characterization reveals that an increase of either electron-doping or hole-doping induced ferromagnetic order in this antiferromagnetic compound, and leads to an insulator-to-metal transition with colossal magnetoresistance showing electron-hole asymmetry. These findings are supported by density functional theory calculations, showing that strengthening of the inter-plane ferromagnetic exchange interaction is the origin of the ambipolar ferromagnetism. The result raises the prospect of exploiting ambipolar magnetic functionality in strongly correlated electron systems.

Direct observation of a two-dimensional hole gas at oxide interfaces.

The discovery of a two-dimensional electron gas (2DEG) at the LaAlO3/SrTiO3 interface 1 has resulted in the observation of many properties2-5 not present in conventional semiconductor heterostructures, and so become a focal point for device applications6-8. Its counterpart, the two-dimensional hole gas (2DHG), is expected to complement the 2DEG. However, although the 2DEG has been widely observed 9 , the 2DHG has proved elusive. Herein we demonstrate a highly mobile 2DHG in epitaxially grown SrTiO3/LaAlO3/SrTiO3 heterostructures. Using electrical transport measurements and in-line electron holography, we provide direct evidence of a 2DHG that coexists with a 2DEG at complementary heterointerfaces in the same structure. First-principles calculations, coherent Bragg rod analysis and depth-resolved cathodoluminescence spectroscopy consistently support our finding that to eliminate ionic point defects is key to realizing a 2DHG. The coexistence of a 2DEG and a 2DHG in a single oxide heterostructure provides a platform for the exciting physics of confined electron-hole systems and for developing applications.

Complex band structure of topological insulator Bi2Se3.

Topological insulators are very interesting from a fundamental point of view, and their unique properties may be useful for electronic and spintronic device applications. From the point of view of applications it is important to understand the decay behavior of carriers injected in the band gap of the topological insulator, which is determined by its complex band structure (CBS). Using first-principles calculations, we investigate the dispersion and symmetry of the complex bands of Bi2Se3 family of three-dimensional topological insulators. We compare the CBS of a band insulator and a topological insulator and follow the CBS evolution in both when the spin-orbit interaction is turned on. We find significant differences in the CBS linked to the topological band structure. In particular, our results demonstrate that the evanescent states in Bi2Se3 are non-trivially complex, i.e. contain both the real and imaginary contributions. This explains quantitatively the oscillatory behavior of the band gap obtained from Bi2Se3 (0 0 0 1) slab calculations.

Giant Enhancement of Magnetic Anisotropy in Ultrathin Manganite Films via Nanoscale 1D Periodic Depth Modulation.

The relatively low magnetocrystalline anisotropy (MCA) in strongly correlated manganites (La,Sr)MnO_{3} has been a major hurdle for implementing them in spintronic applications. Here we report an unusual, giant enhancement of in-plane MCA in 6 nm La_{0.67}Sr_{0.33}MnO_{3} (LSMO) films grown on (001) SrTiO_{3} substrates when the top 2 nm is patterned into periodic stripes of 100 or 200 nm width. Planar Hall effect measurements reveal an emergent uniaxial anisotropy superimposed on one of the original biaxial easy axes for unpatterned LSMO along ⟨110⟩ directions, with a 50-fold enhanced anisotropy energy density of 5.6×10^{6} erg/cm^{3} within the nanostripes, comparable to the value for cobalt. The magnitude and direction of the uniaxial anisotropy exclude shape anisotropy and the step edge effect as its origin. High resolution transmission electron microscopy studies reveal a nonequilibrium strain distribution and drastic suppression in the c-axis lattice constant within the nanostructures, which is the driving mechanism for the enhanced uniaxial MCA, as suggested by first-principles density functional calculations.

Emergence of room-temperature ferroelectricity at reduced dimensions.

The enhancement of the functional properties of materials at reduced dimensions is crucial for continuous advancements in nanoelectronic applications. Here, we report that the scale reduction leads to the emergence of an important functional property, ferroelectricity, challenging the long-standing notion that ferroelectricity is inevitably suppressed at the scale of a few nanometers. A combination of theoretical calculations, electrical measurements, and structural analyses provides evidence of room-temperature ferroelectricity in strain-free epitaxial nanometer-thick films of otherwise nonferroelectric strontium titanate (SrTiO3). We show that electrically induced alignment of naturally existing polar nanoregions is responsible for the appearance of a stable net ferroelectric polarization in these films. This finding can be useful for the development of low-dimensional material systems with enhanced functional properties relevant to emerging nanoelectronic devices.

MAGNETISM. Imaging and control of ferromagnetism in LaMnO3/SrTiO3 heterostructures.

Oxide heterostructures often exhibit unusual physical properties that are absent in the constituent bulk materials. Here, we report an atomically sharp transition to a ferromagnetic phase when polar antiferromagnetic LaMnO3 (001) films are grown on SrTiO3 substrates. For a thickness of six unit cells or more, the LaMnO3 film abruptly becomes ferromagnetic over its entire area, which is visualized by scanning superconducting quantum interference device microscopy. The transition is explained in terms of electronic reconstruction originating from the polar nature of the LaMnO3 (001) films. Our results demonstrate that functionalities can be engineered in oxide films that are only a few atomic layers thick.

Effect of epitaxial strain on tunneling electroresistance in ferroelectric tunnel junctions.

We report the effect of compressive strain on the tunneling electroresistance (TER) effect in BaTiO3/SrRuO3 (BTO/SRO) heterostructures. We find that epitaxial strain imposed by the mismatch of NdGaO3 and SrTiO3 lattice parameters with the BTO and SRO layers improves ferroelectric polarization of BTO and concurrently promotes the metallicity of the SRO films. While the enhanced polarization is beneficial for the TER magnitude, the reduced asymmetry in the tunneling barrier due to the shortened screening length of SRO is detrimental for the effect. Thus, a combined effect of strain on the polarization of the ferroelectric barrier and the screening properties of the electrodes needs to be taken into account when considering and predicting the TER effect in ferroelectric tunnel junctions.

Mechanical Tuning of LaAlO3/SrTiO3 Interface Conductivity.

In recent years, complex-oxide heterostructures and their interfaces have become the focus of significant research activity, primarily driven by the discovery of emerging states and functionalities that open up opportunities for the development of new oxide-based nanoelectronic devices. The highly conductive state at the interface between insulators LaAlO3 and SrTiO3 is a prime example of such emergent functionality, with potential application in high electron density transistors. In this report, we demonstrate a new paradigm for voltage-free tuning of LaAlO3/SrTiO3 (LAO/STO) interface conductivity, which involves the mechanical gating of interface conductance through stress exerted by the tip of a scanning probe microscope. The mechanical control of channel conductivity and the long retention time of the induced resistance states enable transistor functionality with zero gate voltage.

Ferroelectric tunnel junctions with graphene electrodes.

Polarization-driven resistive switching in ferroelectric tunnel junctions (FTJs)--structures composed of two electrodes separated by an ultrathin ferroelectric barrier--offers new physics and materials functionalities, as well as exciting opportunities for the next generation of non-volatile memories and logic devices. Performance of FTJs is highly sensitive to the electrical boundary conditions, which can be controlled by electrode material and/or interface engineering. Here, we demonstrate the use of graphene as electrodes in FTJs that allows control of interface properties for significant enhancement of device performance. Ferroelectric polarization stability and resistive switching are strongly affected by a molecular layer at the graphene/BaTiO3 interface. For the FTJ with the interfacial ammonia layer we find an enhanced tunnelling electroresistance (TER) effect of 6 × 10(5)%. The obtained results demonstrate a new approach based on using graphene electrodes for interface-facilitated polarization stability and enhancement of the TER effect, which can be exploited in the FTJ-based devices.

Long-range electronic reconstruction to a dxz,yz-dominated Fermi surface below the LaAlO3/SrTiO3 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 LaAlO3/SrTiO3 heterostructures at previously unexplored carrier densities n(2D) ≥ 6.9 × 10(14) cm(-2), we observe a Shubnikov-de Haas effect for small in-plane fields, characteristic of an anisotropic 3D Fermi surface with preferential dxz,yz orbital occupancy extending over at least 100 nm perpendicular to the interface. Quantum oscillations from the 3D Fermi surface of bulk doped SrTiO3 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.

Enhanced tunnelling electroresistance effect due to a ferroelectrically induced phase transition at a magnetic complex oxide interface.

The range of recently discovered phenomena in complex oxide heterostructures, made possible owing to advances in fabrication techniques, promise new functionalities and device concepts. One issue that has received attention is the bistable electrical modulation of conductivity in ferroelectric tunnel junctions (FTJs) in response to a ferroelectric polarization of the tunnelling barrier, a phenomenon known as the tunnelling electroresistance (TER) effect. Ferroelectric tunnel junctions with ferromagnetic electrodes allow ferroelectric control of the tunnelling spin polarization through the magnetoelectric coupling at the ferromagnet/ferroelectric interface. Here we demonstrate a significant enhancement of TER due to a ferroelectrically induced phase transition at a magnetic complex oxide interface. Ferroelectric tunnel junctions consisting of BaTiO3 tunnelling barriers and La(0.7)Sr(0.3)MnO3 electrodes exhibit a TER enhanced by up to ~10,000% by a nanometre-thick La(0.5)Ca(0.5)MnO3 interlayer inserted at one of the interfaces. The observed phenomenon originates from the metal-to-insulator phase transition in La(0.5)Ca(0.5)MnO3, driven by the modulation of carrier density through ferroelectric polarization switching. Electrical, ferroelectric and magnetoresistive measurements combined with first-principles calculations provide evidence for a magnetoelectric origin of the enhanced TER, and indicate the presence of defect-mediated conduction in the FTJs. The effect is robust and may serve as a viable route for electronic and spintronic applications.

Mechanically-induced resistive switching in ferroelectric tunnel junctions.

Recent advances in atomic-precision processing of oxide ferroelectrics-materials with a stable polarization that can be switched by an external electric field-have generated considerable interest due to rich physics associated with their fundamental properties and high potential for application in devices with enhanced functionality. One of the particularly promising phenomena is the tunneling electroresistance (TER) effect-polarization-dependent bistable resistance behavior of ferroelectric tunnel junctions (FTJ). Conventionally, the application of an electric field above the coercive field of the ferroelectric barrier is required to observe this phenomenon. Here, we report a mechanically induced TER effect in ultrathin ferroelectric films of BaTiO(3) facilitated by a large strain gradient induced by a tip of a scanning probe microscope (SPM). The obtained results represent a new paradigm for voltage-free control of electronic properties of nanoscale ferroelectrics and, more generally, complex oxide materials.

Ferroelectric tunnel memristor.

Strong interest in resistive switching phenomena is driven by a possibility to develop electronic devices with novel functional properties not available in conventional systems. Bistable resistive devices are characterized by two resistance states that can be switched by an external voltage. Recently, memristors-electric circuit elements with continuously tunable resistive behavior-have emerged as a new paradigm for nonvolatile memories and adaptive electronic circuit elements. Employment of memristors can radically enhance the computational power and energy efficiency of electronic systems. Most of the existing memristor prototypes involve transition metal oxide resistive layers where conductive filaments formation and/or the interface contact resistance control the memristive behavior. In this paper, we demonstrate a new type of memristor that is based on a ferroelectric tunnel junction, where the tunneling conductance can be tuned in an analogous manner by several orders of magnitude by both the amplitude and the duration of the applied voltage. The ferroelectric tunnel memristors exhibit a reversible hysteretic nonvolatile resistive switching with a resistance ratio of up to 10(5) % at room temperature. The observed memristive behavior is attributed to the field-induced charge redistribution at the ferroelectric/electrode interface, resulting in the modulation of the interface barrier height.

Tunable ferroelectricity in artificial tri-layer superlattices comprised of non-ferroic components.

Heterostructured material systems devoid of ferroic components are presumed not to display ordering associated with ferroelectricity. In heterostructures composed of transition metal oxides, however, the disruption introduced by an interface can affect the balance of the competing interactions among electronic spins, charges and orbitals. This has led to the emergence of properties absent in the original building blocks of a heterostructure, including metallicity, magnetism and superconductivity. Here we report the discovery of ferroelectricity in artificial tri-layer superlattices consisting solely of non-ferroelectric NdMnO(3)/SrMnO(3)/LaMnO(3) layers. Ferroelectricity was observed below 40 K exhibiting strong tunability by superlattice periodicity. Furthermore, magnetoelectric coupling resulted in 150% magnetic modulation of the polarization. Density functional calculations indicate that broken space inversion symmetry and mixed valency, because of cationic asymmetry and interfacial polar discontinuity, respectively, give rise to the observed behaviour. Our results demonstrate the engineering of asymmetric layered structures with emergent ferroelectric and magnetic field tunable functions distinct from that of normal devices, for which the components are typically ferroelectrics.