Superfluid stiffness of a KTaO3-based two-dimensional electron gas.

After almost twenty years of intense work on the celebrated LaAlO3/SrTiO3system, the recent discovery of a superconducting two-dimensional electron gas (2-DEG) in (111)-oriented KTaO3-based heterostructures injects new momentum to the field of oxides interface. However, while both interfaces share common properties, experiments also suggest important differences between the two systems. Here, we report gate tunable superconductivity in 2-DEGs generated at the surface of a (111)-oriented KTaO3 crystal by the simple sputtering of a thin Al layer. We extract the superfluid stiffness of the 2-DEGs and show that its temperature dependence is consistent with a node-less superconducting order parameter having a gap value larger than expected within a simple BCS weak-coupling limit model. The superconducting transition follows the Berezinskii-Kosterlitz-Thouless scenario, which was not reported on SrTiO3-based interfaces. Our finding offers innovative perspectives for fundamental science but also for device applications in a variety of fields such as spin-orbitronics and topological electronics.

Large intrinsic anomalous Hall effect in SrIrO3 induced by magnetic proximity effect.

The anomalous Hall effect (AHE) is an intriguing transport phenomenon occurring typically in ferromagnets as a consequence of broken time reversal symmetry and spin-orbit interaction. It can be caused by two microscopically distinct mechanisms, namely, by skew or side-jump scattering due to chiral features of the disorder scattering, or by an intrinsic contribution directly linked to the topological properties of the Bloch states. Here we show that the AHE can be artificially engineered in materials in which it is originally absent by combining the effects of symmetry breaking, spin orbit interaction and proximity-induced magnetism. In particular, we find a strikingly large AHE that emerges at the interface between a ferromagnetic manganite (La0.7Sr0.3MnO3) and a semimetallic iridate (SrIrO3). It is intrinsic and originates in the proximity-induced magnetism present in the narrow bands of strong spin-orbit coupling material SrIrO3, which yields values of anomalous Hall conductivity and Hall angle as high as those observed in bulk transition-metal ferromagnets. These results demonstrate the interplay between correlated electron physics and topological phenomena at interfaces between 3d ferromagnets and strong spin-orbit coupling 5d oxides and trace an exciting path towards future topological spintronics at oxide interfaces.

Antiferromagnetic textures in BiFeO3 controlled by strain and electric field.

Antiferromagnetic thin films are currently generating considerable excitement for low dissipation magnonics and spintronics. However, while tuneable antiferromagnetic textures form the backbone of functional devices, they are virtually unknown at the submicron scale. Here we image a wide variety of antiferromagnetic spin textures in multiferroic BiFeO3 thin films that can be tuned by strain and manipulated by electric fields through room-temperature magnetoelectric coupling. Using piezoresponse force microscopy and scanning NV magnetometry in self-organized ferroelectric patterns of BiFeO3, we reveal how strain stabilizes different types of non-collinear antiferromagnetic states (bulk-like and exotic spin cycloids) as well as collinear antiferromagnetic textures. Beyond these local-scale observations, resonant elastic X-ray scattering confirms the existence of both types of spin cycloids. Finally, we show that electric-field control of the ferroelectric landscape induces transitions either between collinear and non-collinear states or between different cycloids, offering perspectives for the design of reconfigurable antiferromagnetic spin textures on demand.

Inverse transition of labyrinthine domain patterns in ferroelectric thin films.

Phase separation is a cooperative process, the kinetics of which underpin the orderly morphogenesis of domain patterns on mesoscopic scales1,2. Systems of highly degenerate frozen states may exhibit the rare and counterintuitive inverse-symmetry-breaking phenomenon3. Proposed a century ago4, inverse transitions have been found experimentally in disparate materials, ranging from polymeric and colloidal compounds to high-transition-temperature superconductors, proteins, ultrathin magnetic films, liquid crystals and metallic alloys5,6, with the notable exception of ferroelectric oxides, despite extensive theoretical and experimental work on the latter. Here we show that following a subcritical quench, the non-equilibrium self-assembly of ferroelectric domains in ultrathin films of Pb(Zr0.4Ti0.6)O3 results in a maze, or labyrinthine pattern, featuring meandering stripe domains. Furthermore, upon increasing the temperature, this highly degenerate labyrinthine phase undergoes an inverse transition whereby it transforms into the less-symmetric parallel-stripe domain structure, before the onset of paraelectricity at higher temperatures. We find that this phase sequence can be ascribed to an enhanced entropic contribution of domain walls, and that domain straightening and coarsening is predominantly driven by the relaxation and diffusion of topological defects. Computational modelling and experimental observation of the inverse dipolar transition in BiFeO3 suggest the universality of the phenomenon in ferroelectric oxides. The multitude of self-patterned states and the various topological defects that they embody may be used beyond current domain and domain-wall-based7 technologies by enabling fundamentally new design principles and topologically enhanced functionalities within ferroelectric films.

Author Correction: Electric and antiferromagnetic chiral textures at multiferroic domain walls.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Electric and antiferromagnetic chiral textures at multiferroic domain walls.

Chirality, a foundational concept throughout science, may arise at ferromagnetic domain walls1 and in related objects such as skyrmions2. However, chiral textures should also exist in other types of ferroic materials, such as antiferromagnets, for which theory predicts that they should move faster for lower power3, and ferroelectrics, where they should be extremely small and possess unusual topologies4,5. Here, we report the concomitant observation of antiferromagnetic and electric chiral textures at domain walls in the room-temperature ferroelectric antiferromagnet BiFeO3. Combining reciprocal and real-space characterization techniques, we reveal the presence of periodic chiral antiferromagnetic objects along the domain walls as well as a priori energetically unfavourable chiral ferroelectric domain walls. We discuss the mechanisms underlying their formation and their relevance for electrically controlled topological oxide electronics and spintronics.

Competition between electron pairing and phase coherence in superconducting interfaces.

In LaAlO3/SrTiO3 heterostructures, a gate tunable superconducting electron gas is confined in a quantum well at the interface between two insulating oxides. Remarkably, the gas coexists with both magnetism and strong Rashba spin-orbit coupling. However, both the origin of superconductivity and the nature of the transition to the normal state over the whole doping range remain elusive. Here we use resonant microwave transport to extract the superfluid stiffness and the superconducting gap energy of the LaAlO3/SrTiO3 interface as a function of carrier density. We show that the superconducting phase diagram of this system is controlled by the competition between electron pairing and phase coherence. The analysis of the superfluid density reveals that only a very small fraction of the electrons condenses into the superconducting state. We propose that this corresponds to the weak filling of high-energy dxz/dyz bands in the quantum well, more apt to host superconductivity.

Real-space imaging of non-collinear antiferromagnetic order with a single-spin magnetometer.

Although ferromagnets have many applications, their large magnetization and the resulting energy cost for switching magnetic moments bring into question their suitability for reliable low-power spintronic devices. Non-collinear antiferromagnetic systems do not suffer from this problem, and often have extra functionalities: non-collinear spin order may break space-inversion symmetry and thus allow electric-field control of magnetism, or may produce emergent spin-orbit effects that enable efficient spin-charge interconversion. To harness these traits for next-generation spintronics, the nanoscale control and imaging capabilities that are now routine for ferromagnets must be developed for antiferromagnetic systems. Here, using a non-invasive, scanning single-spin magnetometer based on a nitrogen-vacancy defect in diamond, we demonstrate real-space visualization of non-collinear antiferromagnetic order in a magnetic thin film at room temperature. We image the spin cycloid of a multiferroic bismuth ferrite (BiFeO3) thin film and extract a period of about 70 nanometres, consistent with values determined by macroscopic diffraction. In addition, we take advantage of the magnetoelectric coupling present in BiFeO3 to manipulate the cycloid propagation direction by an electric field. Besides highlighting the potential of nitrogen-vacancy magnetometry for imaging complex antiferromagnetic orders at the nanoscale, these results demonstrate how BiFeO3 can be used in the design of reconfigurable nanoscale spin textures.

Strain and Magnetic Field Induced Spin-Structure Transitions in Multiferroic BiFeO3.

The magnetic-field-dependent spin ordering of strained BiFeO3 films is determined using nuclear resonant scattering and Raman spectroscopy. The critical field required to destroy the cycloidal modulation of the Fe spins is found to be significantly lower than in the bulk, with appealing implications for field-controlled spintronic and magnonic devices.

Highly efficient and tunable spin-to-charge conversion through Rashba coupling at oxide interfaces.

The spin-orbit interaction couples the electrons' motion to their spin. As a result, a charge current running through a material with strong spin-orbit coupling generates a transverse spin current (spin Hall effect, SHE) and vice versa (inverse spin Hall effect, ISHE). The emergence of SHE and ISHE as charge-to-spin interconversion mechanisms offers a variety of novel spintronic functionalities and devices, some of which do not require any ferromagnetic material. However, the interconversion efficiency of SHE and ISHE (spin Hall angle) is a bulk property that rarely exceeds ten percent, and does not take advantage of interfacial and low-dimensional effects otherwise ubiquitous in spintronic hetero- and mesostructures. Here, we make use of an interface-driven spin-orbit coupling mechanism-the Rashba effect-in the oxide two-dimensional electron system (2DES) LaAlO3/SrTiO3 to achieve spin-to-charge conversion with unprecedented efficiency. Through spin pumping, we inject a spin current from a NiFe film into the oxide 2DES and detect the resulting charge current, which can be strongly modulated by a gate voltage. We discuss the amplitude of the effect and its gate dependence on the basis of the electronic structure of the 2DES and highlight the importance of a long scattering time to achieve efficient spin-to-charge interconversion.

Tunnel electroresistance through organic ferroelectrics.

Organic electronics is emerging for large-area applications such as photovoltaic cells, rollable displays or electronic paper. Its future development and integration will require a simple, low-power organic memory, that can be written, erased and readout electrically. Here we demonstrate a non-volatile memory in which the ferroelectric polarisation state of an organic tunnel barrier encodes the stored information and sets the readout tunnel current. We use high-sensitivity piezoresponse force microscopy to show that films as thin as one or two layers of ferroelectric poly(vinylidene fluoride) remain switchable with low voltages. Submicron junctions based on these films display tunnel electroresistance reaching 1,000% at room temperature that is driven by ferroelectric switching and explained by electrostatic effects in a direct tunnelling regime. Our findings provide a path to develop low-cost, large-scale arrays of organic ferroelectric tunnel junctions on silicon or flexible substrates.

Hybridization-controlled charge transfer and induced magnetism at correlated oxide interfaces.

At interfaces between conventional materials, band bending and alignment are classically controlled by differences in electrochemical potential. Applying this concept to oxides in which interfaces can be polar and cations may adopt a mixed valence has led to the discovery of novel two-dimensional states between simple band insulators such as LaAlO3 and SrTiO3. However, many oxides have a more complex electronic structure, with charge, orbital and/or spin orders arising from strong Coulomb interactions between transition metal and oxygen ions. Such electronic correlations offer a rich playground to engineer functional interfaces but their compatibility with the classical band alignment picture remains an open question. Here we show that beyond differences in electron affinities and polar effects, a key parameter determining charge transfer at correlated oxide interfaces is the energy required to alter the covalence of the metal-oxygen bond. Using the perovskite nickelate (RNiO3) family as a template, we probe charge reconstruction at interfaces with gadolinium titanate GdTiO3. X-ray absorption spectroscopy shows that the charge transfer is thwarted by hybridization effects tuned by the rare-earth (R) size. Charge transfer results in an induced ferromagnetic-like state in the nickelate, exemplifying the potential of correlated interfaces to design novel phases. Further, our work clarifies strategies to engineer two-dimensional systems through the control of both doping and covalence.

Large elasto-optic effect and reversible electrochromism in multiferroic BiFeO3.

The control of optical fields is usually achieved through the electro-optic or acousto-optic effect in single-crystal ferroelectric or polar compounds such as LiNbO3 or quartz. In recent years, tremendous progress has been made in ferroelectric oxide thin film technology-a field which is now a strong driving force in areas such as electronics, spintronics and photovoltaics. Here, we apply epitaxial strain engineering to tune the optical response of BiFeO3 thin films, and find a very large variation of the optical index with strain, corresponding to an effective elasto-optic coefficient larger than that of quartz. We observe a concomitant strain-driven variation in light absorption--reminiscent of piezochromism--which we show can be manipulated by an electric field. This constitutes an electrochromic effect that is reversible, remanent and not driven by defects. These findings broaden the potential of multiferroics towards photonics and thin film acousto-optic devices, and suggest exciting device opportunities arising from the coupling of ferroic, piezoelectric and optical responses.

Field-effect control of superconductivity and Rashba spin-orbit coupling in top-gated LaAlO3/SrTiO3 devices.

The recent development in the fabrication of artificial oxide heterostructures opens new avenues in the field of quantum materials by enabling the manipulation of the charge, spin and orbital degrees of freedom. In this context, the discovery of two-dimensional electron gases (2-DEGs) at LaAlO3/SrTiO3 interfaces, which exhibit both superconductivity and strong Rashba spin-orbit coupling (SOC), represents a major breakthrough. Here, we report on the realisation of a field-effect LaAlO3/SrTiO3 device, whose physical properties, including superconductivity and SOC, can be tuned over a wide range by a top-gate voltage. We derive a phase diagram, which emphasises a field-effect-induced superconductor-to-insulator quantum phase transition. Magneto-transport measurements show that the Rashba coupling constant increases linearly with the interfacial electric field. Our results pave the way for the realisation of mesoscopic devices, where these two properties can be manipulated on a local scale by means of top-gates.

Local electrical control of magnetic order and orientation by ferroelastic domain arrangements just above room temperature.

Ferroic materials (ferromagnetic, ferroelectric, ferroelastic) usually divide into domains with different orientations of their order parameter. Coupling between different ferroic systems creates new functionalities, for instance the electrical control of macroscopic magnetic properties including magnetization and coercive field. Here we show that ferroelastic domains can be used to control both magnetic order and magnetization direction at the nanoscale with a voltage. We use element-specific X-ray imaging to map the magnetic domains as a function of temperature and voltage in epitaxial FeRh on ferroelastic BaTiO3. Exploiting the nanoscale phase-separation of FeRh, we locally interconvert between ferromagnetic and antiferromagnetic states with a small electric field just above room temperature. Imaging and ab initio calculations show the antiferromagnetic phase of FeRh is favoured by compressive strain on c-oriented BaTiO3 domains, and the resultant magnetoelectric coupling is larger and more reversible than previously reported from macroscopic measurements. Our results emphasize the importance of nanoscale ferroic domain structure and the promise of first-order transition materials to achieve enhanced coupling in artificial multiferroics.

Insight into spin transport in oxide heterostructures from interface-resolved magnetic mapping.

At interfaces between complex oxides, electronic, orbital and magnetic reconstructions may produce states of matter absent from the materials involved, offering novel possibilities for electronic and spintronic devices. Here we show that magnetic reconstruction has a strong influence on the interfacial spin selectivity, a key parameter controlling spin transport in magnetic tunnel junctions. In epitaxial heterostructures combining layers of antiferromagnetic LaFeO(3) (LFO) and ferromagnetic La(0.7)Sr(0.3)MnO(3) (LSMO), we find that a net magnetic moment is induced in the first few unit planes of LFO near the interface with LSMO. Using X-ray photoemission electron microscopy, we show that the ferromagnetic domain structure of the manganite electrodes is imprinted into the antiferromagnetic tunnel barrier, endowing it with spin selectivity. Finally, we find that the spin arrangement resulting from coexisting ferromagnetic and antiferromagnetic interactions strongly influences the tunnel magnetoresistance of LSMO/LFO/LSMO junctions through competing spin-polarization and spin-filtering effects.

Driving Spin Excitations by Hydrostatic Pressure in BiFeO(3).

Optical spectroscopy has been combined with computational and theoretical techniques to show how the spin dynamics in the model multiferroic BiFeO(3) responds to the application of hydrostatic pressure and its corresponding series of structural phase transitions from R3c to the Pnma phases. As pressure increases, multiple spin excitations associated with noncollinear cycloidal magnetism collapse into two excitations, which show jump discontinuities at some of the ensuing crystal phase transitions. The effective Hamiltonian approach provides information on the electrical polarization and structural changes of the oxygen octahedra through the successive structural phases. The extracted parameters are then used in a Ginzburg-Landau model to reproduce the evolution with pressure of the spin wave excitations observed at low energy, and we demonstrate that the structural phases and the magnetic anisotropy drive and control the spin excitations.

Large Elasto-Optic Effect in Epitaxial PbTiO(3) Films.

First-principles calculations are performed to investigate the elasto-optic properties of four different structural phases in (001) epitaxial PbTiO(3) films under tensile strain: a tetragonal (T) phase and an orthorhombic (O) phase, which are the ground states for small and large strain, respectively, and two low-symmetry, monoclinic phases of Cm and Pm symmetries that have low total energy in the intermediate strain range. It is found that the refractive indices of the T and O phases respond differently to epitaxial strain, evidenced by a change of sign of their effective elasto-optic coefficients, and as a result of presently discovered correlations between refractive index, axial ratio, and magnitude of the ferroelectric polarization. The difference in refractive indices between T and O and the existence of such correlations naturally lead to large elasto-optic coefficients in the Cm and Pm states in the intermediate strain range, because Cm structurally bridges the T and O phases (via polarization rotation and a rapid change of its axial ratio) and Pm adopts a similar axial ratio and polarization magnitude to Cm. The present results therefore broaden the palette of functionalities of ferroelectric materials, and suggest new routes to generate systems with unprecedentedly large elasto-optic conversion.

BiFeO3 epitaxial thin films and devices: past, present and future.

The celebrated renaissance of the multiferroics family over the past ten years has also been that of its most paradigmatic member, bismuth ferrite (BiFeO3). Known since the 1960s to be a high temperature antiferromagnet and since the 1970s to be ferroelectric, BiFeO3 only had its bulk ferroic properties clarified in the mid-2000s. It is however the fabrication of BiFeO3 thin films and their integration into epitaxial oxide heterostructures that have fully revealed its extraordinarily broad palette of functionalities. Here we review the first decade of research on BiFeO3 films, restricting ourselves to epitaxial structures. We discuss how thickness and epitaxial strain influence not only the unit cell parameters, but also the crystal structure, illustrated for instance by the discovery of the so-called T-like phase of BiFeO3. We then present its ferroelectric and piezoelectric properties and their evolution near morphotropic phase boundaries. Magnetic properties and their modification by thickness and strain effects, as well as optical parameters, are covered. Finally, we highlight various types of devices based on BiFeO3 in electronics, spintronics, and optics, and provide perspectives for the development of further multifunctional devices for information technology and energy harvesting.

Suppression of the critical thickness threshold for conductivity at the LaAlO3/SrTiO3 interface.

Perovskite materials engineered in epitaxial heterostructures have been intensely investigated during the last decade. The interface formed by an LaAlO3 thin film grown on top of a TiO2-terminated SrTiO3 substrate hosts a two-dimensional electronic system and has become the prototypical example of this field. Although controversy exists regarding some of its physical properties and their precise origin, it is universally found that conductivity only appears beyond an LaAlO3 thickness threshold of four unit cells. Here, we experimentally demonstrate that this critical thickness can be reduced to just one unit cell when a metallic film of cobalt is deposited on top of LaAlO3. First-principles calculations indicate that Co modifies the electrostatic boundary conditions and induces a charge transfer towards the Ti 3d bands, supporting the electrostatic origin of the electronic system at the LaAlO3/SrTiO3 interface. Our results expand the interest of this low-dimensional oxide system from in-plane to perpendicular transport and to the exploration of elastic and inelastic tunnel-type transport of (spin-polarized) carriers.