Size-Dependence and High Temperature Stability of Radial Vortex Magnetic Textures Imprinted by Superconductor Stray Fields.

Swirling spin textures, including topologically nontrivial states, such as skyrmions, chiral domain walls, and magnetic vortices, have garnered significant attention within the scientific community due to their appeal from both fundamental and applied points of view. However, their creation, controlled manipulation, and stability are typically constrained to certain systems with specific crystallographic symmetries, bulk or interface interactions, and/or a precise stacking sequence of materials. Recently, a new approach has shown potential for the imprint of magnetic radial vortices in soft ferromagnetic compounds making use of the stray field of YBa2Cu3O7-δ superconducting microstructures in ferromagnet/superconductor (FM/SC) hybrids at temperatures below the superconducting transition temperature (TC). Here, we explore the lower size limit for the imprint of magnetic radial vortices in square and disc shaped structures as well as the persistence of these spin textures above TC, with magnetic domains retaining partial memory. Structures with circular geometry and with FM patterned to smaller radius than the superconductor island facilitate the imprinting of magnetic radial vortices and improve their stability above TC, in contrast to square structures where the presence of magnetic domains increases the dipolar energy. Micromagnetic modeling coupled with a SC field model reveals that the stabilization mechanism above TC is mediated by microstructural defects. Superconducting control of swirling spin textures, and their stabilization above the superconducting transition temperature by means of defect engineering holds promising prospects for shaping superconducting spintronics based on magnetic textures.

Bimodal ionic photomemristor based on a high-temperature oxide superconductor/semiconductor junction.

Memristors, a cornerstone for neuromorphic electronics, respond to the history of electrical stimuli by varying their electrical resistance across a continuum of states. Much effort has been recently devoted to developing an analogous response to optical excitation. Here we realize a novel tunnelling photo-memristor whose behaviour is bimodal: its resistance is determined by the dual electrical-optical history. This is obtained in a device of ultimate simplicity: an interface between a high-temperature superconductor and a transparent semiconductor. The exploited mechanism is a reversible nanoscale redox reaction between both materials, whose oxygen content determines the electron tunnelling rate across their interface. The redox reaction is optically driven via an interplay between electrochemistry, photovoltaic effects and photo-assisted ion migration. Besides their fundamental interest, the unveiled electro-optic memory effects have considerable technological potential. Especially in combination with high-temperature superconductivity which, in addition to facilitating low-dissipation connectivity, brings photo-memristive effects to the realm of superconducting electronics.

Large Magnetoresistance of Isolated Domain Walls in La2/3 Sr1/3 MnO3 Nanowires.

Generation, manipulation, and sensing of magnetic domain walls are cornerstones in the design of efficient spintronic devices. Half-metals are amenable for this purpose as large low field magnetoresistance signals can be expected from spin accumulation at spin textures. Among half metals, La1- x Srx MnO3 (LSMO) manganites are considered as promising candidates for their robust half-metallic ground state, Curie temperature above room temperature (Tc = 360 K, for x = 1/3), and chemical stability. Yet domain wall magnetoresistance is poorly understood, with large discrepancies in the reported values and conflicting interpretation of experimental data due to the entanglement of various source of magnetoresistance, namely, spin accumulation, anisotropic magnetoresistance, and colossal magnetoresistance. In this work, the domain wall magnetoresistance is measured in LSMO cross-shape nanowires with single-domain walls nucleated across the current path. Magnetoresistance values above 10% are found to be originating at the spin accumulation caused by the mistracking effect of the spin texture of the domain wall by the conduction electrons. Fundamentally, this result shows the importance on non-adiabatic processes at spin textures despite the strong Hund coupling to the localized t2g electrons of the manganite. These large magnetoresistance values are high enough for encoding and reading magnetic bits in future oxide spintronic sensors.

Combining Freestanding Ferroelectric Perovskite Oxides with Two-Dimensional Semiconductors for High Performance Transistors.

We demonstrate the fabrication of field-effect transistors based on single-layer MoS2 and a thin layer of BaTiO3 (BTO) dielectric, isolated from its parent epitaxial template substrate. Thin BTO provides an ultrahigh-κ gate dielectric effectively screening Coulomb scattering centers. These devices show mobilities substantially larger than those obtained with standard SiO2 dielectrics and comparable with values obtained with hexagonal boron nitride, a dielectric employed for fabrication of high-performance two-dimensional (2D) based devices. Moreover, the ferroelectric character of BTO induces a robust hysteresis of the current vs gate voltage characteristics, attributed to its polarization switching. This hysteresis is strongly suppressed when the device is warmed up above the tetragonal-to-cubic transition temperature of BTO that leads to a ferroelectric-to-paraelectric transition. This hysteretic behavior is attractive for applications in memory storage devices. Our results open the door to the integration of a large family of complex oxides exhibiting strongly correlated physics in 2D-based devices.

An Oxygen Vacancy Memristor Ruled by Electron Correlations.

Resistive switching effects offer new opportunities in the field of conventional memories as well as in the booming area of neuromorphic computing. Here the authors demonstrate memristive switching effects produced by a redox-driven oxygen exchange in tunnel junctions based on NdNiO3 , a strongly correlated electron system characterized by the presence of a metal-to-insulator transition (MIT). Strikingly, a strong interplay exists between the MIT and the redox mechanism, which on the one hand modifies the MIT itself, and on the other hand radically affects the tunnel resistance switching and the resistance states' lifetime. That results in a very unique temperature behavior and endows the junctions with multiple degrees of freedom. The obtained results bring up fundamental questions on the interplay between electronic correlations and the creation and mobility of oxygen vacancies in nickelates, opening a new avenue toward mimicking neuromorphic functions by exploiting the electric-field control of correlated states.

Complex structural ordering of the oxygen deficiency in La0.5Ca2.5Mn2O7-δ Ruddlesden-Popper phases.

Ruddlesden-Popper oxides, (AO)(ABO3)n, occupy a prominent place in the landscape of materials research because of their intriguing potential applications. Compositional modifications to the cation sublattices, A or B, have been explored in order to achieve enhanced functionalities. However, changes to the anionic sublattice have been much less explored. In this work, new oxygen-deficient manganese Ruddlesden-Popper-related phases, La0.5Ca2.5Mn2O6.5 and La0.5Ca2.5Mn2O6.25, have been synthesized by controlled reduction of the fully oxidized n = 2 term La0.5Ca2.5Mn2O7. A complete structural and compositional characterization, by means of neutron diffraction, electron diffraction and atomically resolved scanning transmission electron microscopy and electron energy-loss spectroscopy techniques, allows the proposition of a topotactic reduction pathway through preferential oxygen removal in the [MnO2] layers along [031] and [0{\bar 1}3] directions. The gradual decrease of the Mn oxidation state, accommodated by short-range ordering of anionic vacancies, reasonably explains the breaking of ferromagnetic interactions reinforcing the emergence of antiferromagnetic ones. Additional short-range order-disorder phenomena of La and Ca cations have been detected in the reduced La0.5Ca2.5Mn2O7-δ, as previously reported in the parent compound.

Electrically Switchable and Tunable Rashba-Type Spin Splitting in Covalent Perovskite Oxides.

In transition-metal perovskites (ABO_{3}) most physical properties are tunable by structural parameters such as the rotation of the BO_{6} octahedra. Examples include the Néel temperature of orthoferrites, the conductivity of mixed-valence manganites, or the band gap of rare-earth scandates. Since oxides often hold large internal electric dipoles and can accommodate heavy elements, they also emerge as prime candidates to display Rashba spin-orbit coupling, through which charge and spin currents may be efficiently interconverted. However, despite a few experimental reports in SrTiO_{3}-based interface systems, the Rashba interaction has been little studied in these materials, and its interplay with structural distortions remains unknown. In this Letter, we identify a bismuth-based perovskite with a large, electrically switchable Rashba interaction whose amplitude can be controlled by both the ferroelectric polarization and the breathing mode of oxygen octahedra. This particular structural parameter arises from the strongly covalent nature of the Bi-O bonds, reminiscent of the situation in perovskite nickelates. Our results not only provide novel strategies to craft agile spin-charge converters but also highlight the relevance of covalence as a powerful handle to design emerging properties in complex oxides.

A Living-Dead Magnetic Layer at the Surface of Ferrimagnetic DyTiO3 Thin Films.

When ferromagnetic films become ultrathin, key properties such as the Curie temperature and the saturation magnetization are usually depressed. This effect is thoroughly investigated in magnetic oxides such as half-metallic manganites, but much less in ferrimagnetic insulating perovskites such as rare-earth titanates RTiO3 , despite their appeal to design correlated 2D electron gases. Here, the magnetic properties of epitaxial DyTiO3 thin films are reported. While films thicker than about 50 nm show a bulk-like response, at low thickness a surprising increase of the saturation magnetization is observed. This behavior is described using a classical model of a "dead layer" but assuming that this layer is actually "living," that is, it responds to the magnetic field with a strong paramagnetic susceptibility. Through depth-dependent X-ray absorption and photoemission spectroscopy, it is shown that the "living-dead layer" corresponds to surface regions where magnetic (S = 1/2) Ti3+ ions are replaced by nonmagnetic Ti4+ ions. Hysteresis cycles at the Dy M 5 and Ti L 3 edges indicate that the surface Ti4+ ions decouple the Dy3+ ions, thus unleashing their strong paramagnetic response. Finally, it is shown how capping the DyTiO3 film can help increase the Ti3+ content near the surface and thus recover a better ferrimagnetic behavior.

Growth and Electrostatic/chemical Properties of Metal/LaAlO3/SrTiO3 Heterostructures.

The quasi 2D electron system (q2DES) that forms at the interface between LaAlO3 (LAO) and SrTiO3 (STO) has attracted much attention from the oxide electronics community. One of its hallmark features is the existence of a critical LAO thickness of 4 unit-cells (uc) for interfacial conductivity to emerge. Although electrostatic mechanisms have been proposed in the past to describe the existence of this critical thickness, the importance of chemical defects has been recently accentuated. Here, we describe the growth of metal/LAO/STO heterostructures in an ultra-high vacuum (UHV) cluster system combining pulsed laser deposition (to grow the LAO), magnetron sputtering (to grow the metal) and X-ray photoelectron spectroscopy (XPS). We study step by step the formation and evolution of the q2DES and the chemical interactions that occur between the metal and the LAO/STO. Additionally, magnetotransport experiments elucidate on the transport and electronic properties of the q2DES. This systematic work not only demonstrates a way to study the electrostatic and chemical interplay between the q2DES and its environment, but also unlocks the possibility to couple multifunctional capping layers with the rich physics observed in two-dimensional electron systems, allowing the fabrication of new types of devices.

Tuning Up or Down the Critical Thickness in LaAlO3 /SrTiO3 through In Situ Deposition of Metal Overlayers.

The quasi 2D electron system (q2DES) that forms at the interface between LaAlO3 and SrTiO3 has attracted much attention from the oxide electronics community. One of its hallmark features is the existence of a critical LaAlO3 thickness of 4 unit-cells (uc) for interfacial conductivity to emerge. In this paper, the chemical, electronic, and transport properties of LaAlO3 /SrTiO3 samples capped with different metals grown in a system combining pulsed laser deposition, sputtering, and in situ X-ray photoemission spectroscopy are investigated. The results show that for metals with low work function a q2DES forms at 1-2 uc of LaAlO3 and is accompanied by a partial oxidation of the metal, a phenomenon that affects the q2DES properties and triggers the formation of defects. In contrast, for noble metals, the critical thickness is increased above 4 uc. The results are discussed in terms of a hybrid mechanism that incorporates electrostatic and chemical effects.

Resonant electron tunnelling assisted by charged domain walls in multiferroic tunnel junctions.

The peculiar features of domain walls observed in ferroelectrics make them promising active elements for next-generation non-volatile memories, logic gates and energy-harvesting devices. Although extensive research activity has been devoted recently to making full use of this technological potential, concrete realizations of working nanodevices exploiting these functional properties are yet to be demonstrated. Here, we fabricate a multiferroic tunnel junction based on ferromagnetic La0.7Sr0.3MnO3 electrodes separated by an ultrathin ferroelectric BaTiO3 tunnel barrier, where a head-to-head domain wall is constrained. An electron gas stabilized by oxygen vacancies is confined within the domain wall, displaying discrete quantum-well energy levels. These states assist resonant electron tunnelling processes across the barrier, leading to strong quantum oscillations of the electrical conductance.

In operando evidence of deoxygenation in ionic liquid gating of YBa2Cu3O7-X.

Field-effect experiments on cuprates using ionic liquids have enabled the exploration of their rich phase diagrams [Leng X, et al. (2011) Phys Rev Lett 107(2):027001]. Conventional understanding of the electrostatic doping is in terms of modifications of the charge density to screen the electric field generated at the double layer. However, it has been recently reported that the suppression of the metal to insulator transition induced in VO2 by ionic liquid gating is due to oxygen vacancy formation rather than to electrostatic doping [Jeong J, et al. (2013) Science 339(6126):1402-1405]. These results underscore the debate on the true nature, electrostatic vs. electrochemical, of the doping of cuprates with ionic liquids. Here, we address the doping mechanism of the high-temperature superconductor YBa2Cu3O7-X (YBCO) by simultaneous ionic liquid gating and X-ray absorption experiments. Pronounced spectral changes are observed at the Cu K-edge concomitant with the superconductor-to-insulator transition, evidencing modification of the Cu coordination resulting from the deoxygenation of the CuO chains, as confirmed by first-principles density functional theory (DFT) simulations. Beyond providing evidence of the importance of chemical doping in electric double-layer (EDL) gating experiments with superconducting cuprates, our work shows that interfacing correlated oxides with ionic liquids enables a delicate control of oxygen content, paving the way to novel electrochemical concepts in future oxide electronics.

3D elemental mapping with nanometer scale depth resolution via electron optical sectioning.

Electron energy loss spectroscopy in the scanning transmission electron microscope has long been used to perform elemental mapping but has not previously exhibited depth sensitivity. The key to depth resolution with optical sectioning is the transfer of sufficiently high lateral spatial frequencies. By performing spectrum imaging with atomic resolution we achieve nanometer scale depth resolution, enabling us to optically section an oxide heterostructure spectroscopically. Such 3D elemental mapping is sensitive to atomic scale changes in structure and composition and is more interpretable than Z-contrast imaging alone.

Signatures of a two-dimensional ferromagnetic electron gas at the La0.7Sr0.3MnO3/SrTiO3 interface arising from orbital reconstruction.

The magnetoresistance of La0.7Sr0.3MnO3/SrTiO3 superlattices with magnetic field rotating out-of-plane shows unexpected peaks for in-plane fields. Resistivity calculations with spin-orbit coupling reveal that orbital reconstruction at the manganite interface leads to a 2D ferromagnetic electron gas coupled antiparallel to the manganite "bulk". These orbital and magnetic reconstructions are supported by X-ray linear dichroism and ab initio calculations.

Competition between covalent bonding and charge transfer at complex-oxide interfaces.

Here we study the electronic properties of cuprate-manganite interfaces. By means of atomic resolution electron microscopy and spectroscopy, we produce a subnanometer scale map of the transition metal oxidation state profile across the interface between the high Tc superconductor YBa2Cu3O7-δ and the colossal magnetoresistance compound (La,Ca)MnO3. A net transfer of electrons from manganite to cuprate with a peculiar nonmonotonic charge profile is observed. Model calculations rationalize the profile in terms of the competition between standard charge transfer tendencies (due to band mismatch), strong chemical bonding effects across the interface, and Cu substitution into the Mn lattice, with different characteristic length scales.

Oxygen octahedral distortions in LaMO3/SrTiO3 superlattices.

In this work we study the interfaces between the Mott insulator LaMnO3 (LMO) and the band insulator SrTiO3 (STO) in epitaxially grown superlattices with different thickness ratios and different transport and magnetic behaviors. Using atomic resolution electron energy-loss spectral imaging, we analyze simultaneously the structural and chemical properties of these interfaces. We find changes in the oxygen octahedral tilts within the LaMnO3 layers when the thickness ratio between the manganite and the titanate layers is varied. Superlattices with thick LMO and ultrathin STO layers present unexpected octahedral tilts in the STO, along with a small amount of oxygen vacancies. On the other hand, thick STO layers exhibit undistorted octahedra while the LMO layers present reduced O octahedral distortions near the interfaces. These findings are discussed in view of the transport and magnetic differences found in previous studies.

Electron doping by charge transfer at LaFeO3/Sm2CuO4 epitaxial interfaces.

Using X-ray absorption spectroscopy and electron energy loss spectroscopy with atomic-scale spatial resolution, experimental evidence for charge transfer at the interface between the Mott insulators Sm2 CuO4 and LaFeO3 is obtained. As a consequence of the charge transfer, the Sm2 CuO4 is doped with electrons and thus epitaxial Sm2 CuO4 /LaFeO3 heterostructures become metallic.