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Free, publicly-accessible full text available March 12, 2026
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ABSTRACT: Perovskite cobaltites have emerged as archetypes for electrochemical control of materials properties in electrolytegate devices. Voltage-driven redox cycling can be performed between fully oxygenated perovskite and oxygen-vacancy-ordered brownmillerite phases, enabling exceptional modulation of the crystal structure, electronic transport, thermal transport, magnetism, and optical properties. The vast majority of studies, however, have focused heavily on the perovskite and brownmillerite end points. In contrast, here we focus on hysteresis and reversibility across the entire perovskite ↔ brownmillerite topotactic transformation, combining gate-voltage hysteresis loops, minor hysteresis loops, quantitative operando synchrotron X-ray diffraction, and temperature-dependent (magneto)transport, on ion-gel-gated ultrathin (10-unit-cell) epitaxial La0.5Sr0.5CoO3−δ films. Gate-voltage hysteresis loops combined with operando diffraction reveal a wealth of new mechanistic findings, including asymmetric redox kinetics due to differing oxygen diffusivities in the two phases, nonmonotonic transformation rates due to the first-order nature of the transformation, and limits on reversibility due to first-cycle structural degradation. Minor loops additionally enable the first rational design of an optimal gate-voltage cycle. Combining this knowledge, we demonstrate state-of-the-art nonvolatile cycling of electronic and magnetic properties, encompassing >105 transport ON/OFF ratios at room temperature, and reversible metal−insulator−metal and ferromagnet−nonferromagnet−ferromagnet cycling, all at 10-unit-cell thickness with high room-temperature stability. This paves the way for future work to establish the ultimate cycling frequency and endurance of such devices. KEYWORDS: electrolyte gating, magnetoionics, complex oxides, perovskite−brownmillerite transformation, hysteresis, reversibilitymore » « less
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Abstract Contrary to topological insulators, topological semimetals possess a nontrivial chiral anomaly that leads to negative magnetoresistance and are hosts to both conductive bulk states and topological surface states with intriguing transport properties for spintronics. Here, we fabricate highly-ordered metallic Pt3Sn and Pt3SnxFe1-xthin films via sputtering technology. Systematic angular dependence (both in-plane and out-of-plane) study of magnetoresistance presents surprisingly robust quadratic and linear negative longitudinal magnetoresistance features for Pt3Sn and Pt3SnxFe1-x, respectively. We attribute the anomalous negative longitudinal magnetoresistance to the type-II Dirac semimetal phase (pristine Pt3Sn) and/or the formation of tunable Weyl semimetal phases through symmetry breaking processes, such as magnetic-atom doping, as confirmed by first-principles calculations. Furthermore, Pt3Sn and Pt3SnxFe1-xshow the promising performance for facilitating the development of advanced spin-orbit torque devices. These results extend our understanding of chiral anomaly of topological semimetals and can pave the way for exploring novel topological materials for spintronic devices.more » « less
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Abstract As a promising alternative to the mainstream CoFeB/MgO system with interfacial perpendicular magnetic anisotropy (PMA),L10‐FePd and its synthetic antiferromagnet (SAF) structure with large crystalline PMA can support spintronic devices with sufficient thermal stability at sub‐5 nm sizes. However, the compatibility requirement of preparingL10‐FePd thin films on Si/SiO2wafers is still unmet. In this paper, high‐qualityL10‐FePd and its SAF on Si/SiO2wafers are prepared by coating the amorphous SiO2surface with an MgO(001) seed layer. The preparedL10‐FePd single layer and SAF stack are highly (001)‐textured, showing strong PMA, low damping, and sizeable interlayer exchange coupling, respectively. Systematic characterizations, including advanced X‐ray diffraction measurement and atomic resolution‐scanning transmission electron microscopy, are conducted to explain the outstanding performance ofL10‐FePd layers. A fully‐epitaxial growth that starts from MgO seed layer, induces the (001) texture ofL10‐FePd, and extends through the SAF spacer is observed. This study makes the vision of scalable spintronics more practical.more » « less
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