Domain-resolved room-temperature magneto-electric coupling in manganite-titanate heterostructures

We present a model artificial multiferroic system consisting of a (011)-oriented ferroelectric Pb(Mg,Nb,Ti)O$_3$ substrate intimately coupled to a ferromagnetic (La,Sr)MnO$_3$ film through epitaxial strain and converse piezoelectric effects. Electric field pulse sequences of less than 6 kV/cm were shown to induce large reversible and bistable remanent strains in the manganite film. Magnetic hysteresis loops demonstrate that the changes in strain states result in significant changes in magnetic anisotropy from a highly anisotropic two-fold magnetic symmetry to a more isotropic one. Such changes in magnetic anisotropy are reversible upon multiple cycles and are stable at zero applied electric field, and are accompanied by large changes in resistivity. We directly image the change between the two-fold and isotropic magnetic configurations at the scale of a single ferromagnetic domain using X-ray photoemission electron microscopy as a function of applied electric field pulses. Imaging the domain reversal process as a function of electric field shows that the energy barrier for magnetization reversal is drastically lowered, by up to 70% as determined from free energy calculations, through the anisotropic strain change generated by the ferroelectric substrate. Thus, an electric field pulse can be used to 'set' and 'reset' the magnetic anisotropy orientation and resistive state in the film, as well as lowering the coercive field required to reverse magnetization, showing a promising route towards electric-field manipulation of multifunctional nanostructures at room temperature.Comment: 6 figures, 1 tabl

Controlling antiferromagnetic domains in patterned La0.7Sr0.3FeO3 thin films

Transition metal oxide thin films and heterostructures are promising platforms to achieve full control of the antiferromagnetic (AFM) domain structure in patterned features as needed for AFM spintronic devices. In this work, soft x-ray photoemission electron microscopy was utilized to image AFM domains in micromagnets patterned into La0.7Sr0.3FeO3 (LSFO) thin films and La0.7Sr0.3MnO3 (LSMO)/LSFO superlattices. A delicate balance exists between magnetocrystalline anisotropy, shape anisotropy, and exchange interactions such that the AFM domain structure can be controlled using parameters such as LSFO and LSMO layer thickness, micromagnet shape, and temperature. In LSFO thin films, shape anisotropy gains importance only in micromagnets where at least one extended edge is aligned parallel to an AFM easy axis. In contrast, in the limit of ultrathin LSFO layers in the LSMO/LSFO superlattice, shape anisotropy effects dominate such that the AFM spin axes at micromagnet edges can be aligned along any in-plane crystallographic direction

Spin-flop coupling at La0.5Sr0.5FeO3/La0.7Sr0.3MnO3 interfaces

Antiferromagnetic (AFM) spintronics offer several benefits compared to their ferromagnetic (FM) counterparts, such as high storage capacity and faster processing speed, however, difficulties in manipulating and detecting the AFM moments impede their implementation. Spin-flop coupling, the interfacial perpendicular coupling between FM and AFM moments, can be utilized to control the orientation of AFM moments with the application of moderate magnetic fields on the scale of tenths of a Tesla. In this work, epitaxial bilayers of AFM La0.5Sr0.5FeO3 (LSFO)/FM La0.7Sr0.3MnO3 (LSMO) with fixed LSMO thickness (∼85 u.c.) and LSFO thicknesses varying from 10 to 50 u.c. were investigated to determine the effect of Sr doping and La1-xSrxFeO3 magnetocrystalline anisotropy on the strength of spin-flop coupling. X-ray magnetic linear dichroism demonstrated that the spin-flop coupling strength decreased with increasing LSFO layer thickness, persisting at a thickness of 50 u.c. (∼20 nm). Furthermore, photoemission electron microscopy revealed a domain-by-domain correlation between the FM and AFM domains consistent with the perpendicular orientation dictated by spin-flop coupling. These results demonstrate that LSFO/LSMO bilayers have the potential to serve as a model materials system for AFM spin transport measurements

Magnetoresistance anomaly during the electrical triggering of a metal-insulator transition

Phase separation naturally occurs in a variety of magnetic materials and it often has a major impact on both electric and magnetotransport properties. In resistive switching systems, phase separation can be created on demand by inducing local switching, which provides an opportunity to tune the electronic and magnetic state of the device by applying voltage. Here we explore the magnetotransport properties in the ferromagnetic oxide (La,Sr)MnO3 (LSMO) during the electrical triggering of an intrinsic metal-insulator transition (MIT) that produces volatile resistive switching. This switching occurs in a characteristic spatial pattern, i.e., the formation of an insulating barrier perpendicular to the current flow, enabling an electrically actuated ferromagnetic-paramagnetic-ferromagnetic phase separation. At the threshold voltage of the MIT triggering, both anisotropic and colossal magnetoresistances exhibit anomalies including a large increase in magnitude and a sign flip. Computational analysis revealed that these anomalies originate from the coupling between the switching-induced phase separation state and the intrinsic magnetoresistance of LSMO. This work demonstrates that driving the MIT material into an out-of-equilibrium resistive switching state provides the means to electrically control of the magnetotransport phenomena

Voltage-controlled magnetism enabled by resistive switching

The discovery of new mechanisms of controlling magnetic properties by electric fields or currents furthers the fundamental understanding of magnetism and has important implications for practical use. Here, we present a novel approach of utilizing resistive switching to control magnetic anisotropy. We study a ferromagnetic oxide that exhibits an electrically triggered metal-to-insulator phase transition producing a volatile resistive switching. This switching occurs in a characteristic spatial pattern: the formation of a transverse insulating barrier inside a metallic matrix resulting in an unusual ferromagnetic/paramagnetic/ferromagnetic configuration. We found that the formation of this voltage-driven paramagnetic insulating barrier is accompanied by the emergence of a strong uniaxial magnetic anisotropy that overpowers the intrinsic material anisotropy. Our results demonstrate that resistive switching is an effective tool for manipulating magnetic properties. Because resistive switching can be induced in a very broad range of materials, our findings could enable a new class of voltage-controlled magnetism systems

Unusual structural rearrangement and superconductivity in infinite layer cuprate superlattices

Epitaxial stabilization of thermodynamically metastable phases and advances in atomic control of complex oxide thin-film growth can be used effectively for realizing novel phenomena and as an alternative for bulk synthesis under extreme thermodynamic conditions. Here, we investigate infinite layer (IL) based cuprate superlattices, where 7-8 unit cells of Sr0.6Ca0.4CuO2 (SCCO) are sandwiched between ultrathin spacer layers of SrTiO3 (STO), SrRuO3, or BaCuO2 (BCO) and only observe superconductivity in the pure [SCCO/BCO] superlattice (SL) without spacer layers. Apparently, the insertion of an additional STO spacer layer in the latter SL prevents the occurrence of superconductivity. The observed superconductivity in [SCCO/BCO] SL is discussed in terms of a structural model involving the interplay between the CuO2 plane and the CuO chain similar to the bulk YBa2Cu3O7 superconductor. The structural origin was found by the identification of a metastable IL-BaCuO2 variant, which deviates highly from its parent bulk crystal structure and exhibits a relatively larger out-of-plane lattice parameter (around 7Å) when sandwiched with SCCO in the form of [SCCO/BCO] SL. However, this variant is absent when STO spacer layers are introduced between SCCO and BCO layers. X-ray absorption spectra of the Cu L edge for BCO exhibits a slightly higher energy satellite peak as compared to the 3d9L Zhang-Rice character observed in SCCO. This result indicates the existence of contrasting plane and chain-type Cu-O blocks in SCCO and BCO, respectively, which is further corroborated using annular bright field scanning transmission electron microscopy imaging. This work unravels an unexpected structure of BCO which helps in realizing superconductivity in [SCCO/BCO] SL and provides a wider perspective in the growth and design of cuprate-based hybrid structures.</p

Interfacial-Redox-Induced Tuning of Superconductivity in YBa2Cu3O7-δ.

Solid-state ionic approaches for modifying ion distributions in getter/oxide heterostructures offer exciting potentials to control material properties. Here, we report a simple, scalable approach allowing for manipulation of the superconducting transition in optimally doped YBa2Cu3O7-δ (YBCO) films via a chemically driven ionic migration mechanism. Using a thin Gd capping layer of up to 20 nm deposited onto 100 nm thick epitaxial YBCO films, oxygen is found to leach from deep within the YBCO. Progressive reduction of the superconducting transition is observed, with complete suppression possible for a sufficiently thick Gd layer. These effects arise from the combined impact of redox-driven electron doping and modification of the YBCO microstructure due to oxygen migration and depletion. This work demonstrates an effective step toward total ionic tuning of superconductivity in oxides, an interface-induced effect that goes well into the quasi-bulk regime, opening-up possibilities for electric field manipulation

Ionic Tuning of Cobaltites at the Nanoscale

Control of materials through custom design of ionic distributions represents a powerful new approach to develop future technologies ranging from spintronic logic and memory devices to energy storage. Perovskites have shown particular promise for ionic devices due to their high ion mobility and sensitivity to chemical stoichiometry. In this work, we demonstrate a solid-state approach to control of ionic distributions in (La,Sr)CoO$_{3}$ thin films. Depositing a Gd capping layer on the perovskite film, oxygen is controllably extracted from the structure, up-to 0.5 O/u.c. throughout the entire 36 nm thickness. Commensurate with the oxygen extraction, the Co valence state and saturation magnetization show a smooth continuous variation. In contrast, magnetoresistance measurements show no-change in the magnetic anisotropy and a rapid increase in the resistivity over the same range of oxygen stoichiometry. These results suggest significant phase separation, with metallic ferromagnetic regions and oxygen-deficient, insulating, non-ferromagnetic regions, forming percolated networks. Indeed, X-ray diffraction identifies oxygen-vacancy ordering, including transformation to a brownmillerite crystal structure. The unexpected transformation to the brownmillerite phase at ambient temperature is further confirmed by high-resolution scanning transmission electron microscopy which shows significant structural - and correspondingly chemical - phase separation. This work demonstrates room-temperature ionic control of magnetism, electrical resistivity, and crystalline structure in a 36 nm thick film, presenting new opportunities for ionic devices that leverage multiple material functionalities