The first order reversal curve (FORC) method is a magnetometry based technique used to capture nanoscale magnetic phase separation and interactions with macroscopic measurements using minor hysteresis loop analysis. This makes the FORC technique a powerful tool in the analysis of complex systems which cannot be effectively probed using localized techniques. However, recovering quantitative details about the identified phases which can be compared to traditionally measured metrics remains an enigmatic challenge. We demonstrate a technique to reconstruct phase-resolved magnetic hysteresis loops by selectively integrating the measured FORC distribution. From these minor loops, the traditional metrics-including the coercivity and saturation field, and the remanent and saturation magnetization-can be determined. In order to perform this analysis, special consideration must be paid to the accurate quantitative management of the so-called reversible features. This technique is demonstrated on three representative materials systems, high anisotropy FeCuPt thin-films, Fe nanodots, and SmCo/Fe exchange spring magnet films, and shows excellent agreement with the direct measured major loop, as well as the phase separated loops.

Magnetic multilayer thin films with perpendicular magnetic anisotropy (PMA) and interfacial Dzyaloshinskii-Moriya interaction (iDMI) are of intense interest for realizing magnetic skyrmions and modifying topological spin textures. We systematically investigate interlayer exchange coupling (IEC) in Pt/Co/Ru(Ir) superlattices that have PMA and large iDMI. The IEC is greatly tunable by varying Ru(Ir) or Pt thickness and the antiferromagnetic IEC is as large as 1.3mJ/m2 that is on the same order of magnitude as the iDMI. We find unusual magnetic hysteresis loop crossing between field-ascending and -descending magnetization curves. Furthermore, we identify magnetic phase diagrams for antiferromagnetic IEC and hysteresis loop crossing with respect to Ru(Ir) and Pt thickness. Our experimental findings may open a way in the development of synthetic antiferromagnetic spintronics and/or the realization of antiferromagnetic skyrmions.

Electrically induced ionic motion offers a new way to realize voltage-controlled magnetism, opening the door to a new generation of logic, sensor, and data storage technologies. Here, we demonstrate an effective approach to magneto-ionically and electrically tune the exchange bias in Gd/Ni_1-xCo_xO thin films (x = 0.50 and 0.67), where neither of the layers alone is ferromagnetic at room temperature. The Gd capping layer deposited onto antiferromagnetic Ni_1-xCo_xO initiates a solid-state redox reaction that reduces an interfacial region of the oxide to ferromagnetic NiCo. An exchange bias is established after field cooling (FC), which can be enhanced by up to 35% after a voltage conditioning and subsequently reset with a second FC. These effects are caused by the presence of an interfacial ferromagnetic NiCo layer, which further alloys with the Gd layer upon FC and voltage application, as confirmed by electron microscopy and polarized neutron reflectometry studies. These results highlight the viability of the solid-state magneto-ionic approach to achieve electric control of exchange bias, with potential for energy-efficient magneto-ionic devices.

Magnetoelectric coupling in ferromagnetic/multiferroic systems is often manifested in the exchange bias effect, which may have combined contributions from multiple sources, such as domain walls, chemical defects, or strain. In this study we magnetically "fingerprint" the coupling behavior of CoFe grown on epitaxial BiFeO3 (BFO) thin films by magnetometry and the first-order-reversal-curves (FORC). The contribution to exchange bias from 71°, 109° and charged ferroelectric domain walls (DWs) was elucidated by the FORC distribution. CoFe samples grown on BFO with 71° DWs only exhibit an enhancement of the coercivity, but little exchange bias. Samples grown on BFO with 109° DWs and mosaic DWs exhibit a much larger exchange bias, with the main enhancement attributed to 109° and charged DWs. Based on the Malozemoff random field model, a varying-anisotropy model is proposed to account for the exchange bias enhancement. This work sheds light on the relationship between the exchange bias effect of the CoFe/BFO heterointerface and the ferroelectric DWs, and provides a path for multiferroic device analysis and design.

Free-standing, interconnected metallic nanowire networks with densities as low as 40 mg/cm³ have been achieved over centimeter-scale areas, using electrodeposition into polycarbonate membranes that have been ion-tracked at multiple angles. Networks of interconnected magnetic nanowires further provide an exciting platform to explore 3-dimensional nanomagnetism, where their structure, topology, and frustration may be used as additional degrees of freedom to tailor the materials properties. New magnetization reversal mechanisms in cobalt networks are captured by the first-order reversal curve method, which demonstrate the evolution from strong demagnetizing dipolar interactions to intersection-mediated domain wall pinning and propagation, and eventually to shape-anisotropy dominated magnetization reversal. These findings open up new possibilities for 3-dimensional integrated magnetic devices for memory, complex computation, and neuromorphics.

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 YBa₂Cu₃O_7-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.

Remanence magnetization plots (e.g., Henkel or δM plots) have been extensively used as a straightforward way to determine the presence and intensity of dipolar and exchange interactions in assemblies of magnetic nanoparticles or single domain grains. Their evaluation is particularly important in functional materials whose performance is strongly affected by the intensity of interparticle interactions, such as patterned recording media and nanostructured permanent magnets, as well as in applications such as hyperthermia and magnetic resonance imaging. Here, we demonstrate that δM plots may be misleading when the nanoparticles do not have a homogeneous internal magnetic configuration. Substantial dips in the M plots of γ-Fe2O3 nanoparticles isolated by thick SiO2 shells indicate the presence of demagnetizing interactions, usually identified as dipolar interactions. Our results, however, demonstrate that it is the inhomogeneous spin structure of the nanoparticles, as most clearly evidenced by Mössbauer measurements, that has a pronounced effect on the δM plots, leading to features remarkably similar to those produced by dipolar interactions. X-ray diffraction results combined with magnetic characterization indicate that this inhomogeneity is due to the presence of surface structural (and spin) disorder. Monte Carlo simulations unambiguously corroborate the critical role of the internal magnetic structure in the δM plots. Our findings constitute a cautionary tale on the widespread use of remanence plots to assess interparticle interactions as well as offer new perspectives in the use of Henkel and δM plots to quantify the rather elusive inhomogeneous magnetization states in nanoparticles.

Electric-field-controlled magnetism can boost energy efficiency in widespread applications. However, technologically, this effect is facing important challenges: mechanical failure in strain-mediated piezoelectric/magnetostrictive devices, dearth of room-temperature multiferroics, or stringent thickness limitations in electrically charged metallic films. Voltage-driven ionic motion (magneto-ionics) circumvents most of these drawbacks while exhibiting interesting magnetoelectric phenomena. Nevertheless, magneto-ionics typically requires heat treatments and multicomponent heterostructures. Here we report on the electrolyte-gated and defect-mediated O and Co transport in a Co₃O₄ single layer which allows for room-temperature voltage-controlled ON-OFF ferromagnetism (magnetic switch) via internal reduction/oxidation processes. Negative voltages partially reduce Co₃O₄ to Co (ferromagnetism: ON), resulting in graded films including Co- and O-rich areas. Positive bias oxidizes Co back to Co₃O₄ (paramagnetism: OFF). This electric-field-induced atomic-scale reconfiguration process is compositionally, structurally, and magnetically reversible and self-sustained, since no oxygen source other than the Co₃O₄ itself is required. This process could lead to electric-field-controlled device concepts for spintronics.

Complex oxide heterostructures provide access to emergent functional and structural phases which are not present in the bulk constituent materials. In this Rapid Communication, we focus on La0.67Sr0.33CoO3 (LSCO)/Gd heterostructures due to the high oxygen ion conductivity, as well as the coupled magnetic and electronic properties of LSCO, which are strongly dependent on the oxygen stoichiometry. This combination of properties enables the ionic control of the functional properties of LSCO thin films through the presence of oxygen getter layers such as Gd. We utilize X-ray nanodiffraction to directly image the nanoscale morphology of LSCO thin films as they are progressively transformed from the equilibrium perovskite phase to the metastable brownmillerite (BM) phase with increasing Gd thickness. Our studies show the coexistence of perovskite and BM phases with a critical oxygen vacancy concentration threshold which leads to the formation of extended BM filaments. In addition to lateral phase separation, we observed phase separation within the film thickness possibly due to pinning of the perovskite and BM phases by the substrate/LSCO and LSCO/Gd interface, respectively. Our studies provide a nanoscale survey of the phase separation in the cobaltites and shed light on the formation of the metastable BM phase.

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)CoO3 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, nonferromagnetic 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 opportunities for ionic devices that leverage multiple material functionalities.