Coexistence of Superconductivity and Antiferromagnetism in Topological Magnet MnBi2Te4 Films.

The interface of two materials can harbor unexpected emergent phenomena. One example is interface-induced superconductivity. In this work, we employ molecular beam epitaxy to grow a series of heterostructures formed by stacking together two nonsuperconducting antiferromagnetic materials, an intrinsic antiferromagnetic topological insulator MnBi2Te4 and an antiferromagnetic iron chalcogenide FeTe. Our electrical transport measurements reveal interface-induced superconductivity in these heterostructures. By performing scanning tunneling microscopy and spectroscopy measurements, we observe a proximity-induced superconducting gap on the top surface of the MnBi2Te4 layer, confirming the coexistence of superconductivity and antiferromagnetism in the MnBi2Te4 layer. Our findings will advance the fundamental inquiries into the topological superconducting phase in hybrid devices and provide a promising platform for the exploration of chiral Majorana physics in MnBi2Te4-based heterostructures.

Reduction-Induced Magnetic Behavior in LaFeO3-δ Thin Films.

The effect of oxygen reduction on the magnetic properties of LaFeO3-δ (LFO) thin films was studied to better understand the viability of LFO as a candidate for magnetoionic memory. Differences in the amount of oxygen lost by LFO and its magnetic behavior were observed in nominally identical LFO films grown on substrates prepared using different common methods. In an LFO film grown on as-received SrTiO3 (STO) substrate, the original perovskite film structure was preserved following reduction, and remnant magnetization was only seen at low temperatures. In a LFO film grown on annealed STO, the LFO lost significantly more oxygen and the microstructure decomposed into La- and Fe-rich regions with remnant magnetization that persisted up to room temperature. These results demonstrate an ability to access multiple, distinct magnetic states via oxygen reduction in the same starting material and suggest LFO may be a suitable materials platform for nonvolatile multistate memory.

Emergent Ferromagnetism in CaRuO3/CaMnO3 (111)-Oriented Superlattices.

The boundary between CaRuO3 and CaMnO3 is an ideal test bed for emergent magnetic ground states stabilized through interfacial electron interactions. In this system, nominally antiferromagnetic and paramagnetic materials combine to yield interfacial ferromagnetism in CaMnO3 due to electron leakage across the interface. In this work, we show that the crystal symmetry at the surface is a critical factor determining the nature of the interfacial interactions. Specifically, by growing CaRuO3/CaMnO3 heterostructures along the (111) instead of the (001) crystallographic axis, we achieve a 3-fold enhancement of the magnetization and involve the CaRuO3 layers in the ferromagnetism, which now spans both constituent materials. The stabilization of a net magnetic moment in CaRuO3 through strain effects has been long-sought but never consistently achieved, and our observations demonstrate the importance of interface engineering in the development of new functional heterostructures.

Interface-induced superconductivity in magnetic topological insulators.

The interface between two different materials can show unexpected quantum phenomena. In this study, we used molecular beam epitaxy to synthesize heterostructures formed by stacking together two magnetic materials, a ferromagnetic topological insulator (TI) and an antiferromagnetic iron chalcogenide (FeTe). We observed emergent interface-induced superconductivity in these heterostructures and demonstrated the co-occurrence of superconductivity, ferromagnetism, and topological band structure in the magnetic TI layer-the three essential ingredients of chiral topological superconductivity (TSC). The unusual coexistence of ferromagnetism and superconductivity is accompanied by a high upper critical magnetic field that exceeds the Pauli paramagnetic limit for conventional superconductors at low temperatures. These magnetic TI/FeTe heterostructures with robust superconductivity and atomically sharp interfaces provide an ideal wafer-scale platform for the exploration of chiral TSC and Majorana physics.

Exchange-Biased Quantum Anomalous Hall Effect.

The quantum anomalous Hall (QAH) effect is characterized by a dissipationless chiral edge state with a quantized Hall resistance at zero magnetic field. Manipulating the QAH state is of great importance in both the understanding of topological quantum physics and the implementation of dissipationless electronics. Here, the QAH effect is realized in the magnetic topological insulator Cr-doped (Bi,Sb)2 Te3 (CBST) grown on an uncompensated antiferromagnetic insulator Al-doped Cr2 O3 . Through polarized neutron reflectometry (PNR), a strong exchange coupling is found between CBST and Al-Cr2 O3 surface spins fixing interfacial magnetic moments perpendicular to the film plane. The interfacial coupling results in an exchange-biased QAH effect. This study further demonstrates that the magnitude and sign of the exchange bias can be effectively controlled using a field training process to set the magnetization of the Al-Cr2 O3 layer. It demonstrates the use of the exchange bias effect to effectively manipulate the QAH state, opening new possibilities in QAH-based spintronics.

Nitrogen-Based Magneto-ionic Manipulation of Exchange Bias in CoFe/MnN Heterostructures.

Electric field control of the exchange bias effect across ferromagnet/antiferromagnet (FM/AF) interfaces has offered exciting potentials for low-energy-dissipation spintronics. In particular, the solid-state magneto-ionic means is highly appealing as it may allow reconfigurable electronics by transforming the all-important FM/AF interfaces through ionic migration. In this work, we demonstrate an approach that combines the chemically induced magneto-ionic effect with the electric field driving of nitrogen in the Ta/Co0.7Fe0.3/MnN/Ta structure to electrically manipulate exchange bias. Upon field-cooling the heterostructure, ionic diffusion of nitrogen from MnN into the Ta layers occurs. A significant exchange bias of 618 Oe at 300 K and 1484 Oe at 10 K is observed, which can be further enhanced after a voltage conditioning by 5 and 19%, respectively. This enhancement can be reversed by voltage conditioning with an opposite polarity. Nitrogen migration within the MnN layer and into the Ta capping layer cause the enhancement in exchange bias, which is observed in polarized neutron reflectometry studies. These results demonstrate an effective nitrogen-ion based magneto-ionic manipulation of exchange bias in solid-state devices.

Room-temperature valence transition in a strain-tuned perovskite oxide.

Cobalt oxides have long been understood to display intriguing phenomena known as spin-state crossovers, where the cobalt ion spin changes vs. temperature, pressure, etc. A very different situation was recently uncovered in praseodymium-containing cobalt oxides, where a first-order coupled spin-state/structural/metal-insulator transition occurs, driven by a remarkable praseodymium valence transition. Such valence transitions, particularly when triggering spin-state and metal-insulator transitions, offer highly appealing functionality, but have thus far been confined to cryogenic temperatures in bulk materials (e.g., 90 K in Pr1-xCaxCoO3). Here, we show that in thin films of the complex perovskite (Pr1-yYy)1-xCaxCoO3-δ, heteroepitaxial strain tuning enables stabilization of valence-driven spin-state/structural/metal-insulator transitions to at least 291 K, i.e., around room temperature. The technological implications of this result are accompanied by fundamental prospects, as complete strain control of the electronic ground state is demonstrated, from ferromagnetic metal under tension to nonmagnetic insulator under compression, thereby exposing a potential novel quantum critical point.

Engineering Magnetic Anisotropy and Emergent Multidirectional Soft Ferromagnetism in Ultrathin Freestanding LaMnO3 Films.

The combination of small coercive fields and weak magnetic anisotropy makes soft ferromagnetic films extremely useful for nanoscale devices that need to easily switch spin directions. However, soft ferromagnets are relatively rare, particularly in ultrathin films with thicknesses of a few nanometers or less. We have synthesized large-area, high-quality, ultrathin freestanding LaMnO3 films on Si and found unexpected soft ferromagnetism along both the in-plane and out-of-plane directions when the film thickness was reduced to 4 nm. We argue that the vanishing magnetic anisotropy between the two directions is a consequence of two coexisting magnetic easy axes in different atomic layers of the LaMnO3 film. Spectroscopy measurements reveal a change in Mn valence from 3+ in the film interior to approximately 2+ at the surfaces where considerable hydrogen infiltration occurs due to the water dissolving process. First-principles calculations show that protonation of LaMnO3 decreases the Mn valence and switches the magnetic easy axis from in-plane to out-of-plane as the Mn valence approaches 2+ from its 3+ bulk value. Our work demonstrates that ultrathin freestanding films can exhibit functional properties that are absent in homogeneous materials, concomitant with their convenient compatibility with Si-based devices.

Emergent electric field control of phase transformation in oxide superlattices.

Electric fields can transform materials with respect to their structure and properties, enabling various applications ranging from batteries to spintronics. Recently electrolytic gating, which can generate large electric fields and voltage-driven ion transfer, has been identified as a powerful means to achieve electric-field-controlled phase transformations. The class of transition metal oxides provide many potential candidates that present a strong response under electrolytic gating. However, very few show a reversible structural transformation at room-temperature. Here, we report the realization of a digitally synthesized transition metal oxide that shows a reversible, electric-field-controlled transformation between distinct crystalline phases at room-temperature. In superlattices comprised of alternating one-unit-cell of SrIrO3 and La0.2Sr0.8MnO3, we find a reversible phase transformation with a 7% lattice change and dramatic modulation in chemical, electronic, magnetic and optical properties, mediated by the reversible transfer of oxygen and hydrogen ions. Strikingly, this phase transformation is absent in the constituent oxides, solid solutions and larger period superlattices. Our findings open up this class of materials for voltage-controlled functionality.

Ultralow Damping in Nanometer-Thick Epitaxial Spinel Ferrite Thin Films.

Pure spin currents, unaccompanied by dissipative charge flow, are essential for realizing energy-efficient nanomagnetic information and communications devices. Thin-film magnetic insulators have been identified as promising materials for spin-current technology because they are thought to exhibit lower damping compared with their metallic counterparts. However, insulating behavior is not a sufficient requirement for low damping, as evidenced by the very limited options for low-damping insulators. Here, we demonstrate a new class of nanometer-thick ultralow-damping insulating thin films based on design criteria that minimize orbital angular momentum and structural disorder. Specifically, we show ultralow damping in <20 nm thick spinel-structure magnesium aluminum ferrite (MAFO), in which magnetization arises from Fe3+ ions with zero orbital angular momentum. These epitaxial MAFO thin films exhibit a Gilbert damping parameter of ∼0.0015 and negligible inhomogeneous linewidth broadening, resulting in narrow half width at half-maximum linewidths of ∼0.6 mT around 10 GHz. Our findings offer an attractive thin-film platform for enabling integrated insulating spintronics.

Tuning Perpendicular Magnetic Anisotropy by Oxygen Octahedral Rotations in (La_{1-x}Sr_{x}MnO_{3})/(SrIrO_{3}) Superlattices.

Perpendicular magnetic anisotropy (PMA) plays a critical role in the development of spintronics, thereby demanding new strategies to control PMA. Here we demonstrate a conceptually new type of interface induced PMA that is controlled by oxygen octahedral rotation. In superlattices comprised of La_{1-x}Sr_{x}MnO_{3} and SrIrO_{3}, we find that all superlattices (0≤x≤1) exhibit ferromagnetism despite the fact that La_{1-x}Sr_{x}MnO_{3} is antiferromagnetic for x>0.5. PMA as high as 4×10^{6} erg/cm^{3} is observed by increasing x and attributed to a decrease of oxygen octahedral rotation at interfaces. We also demonstrate that oxygen octahedral deformation cannot explain the trend in PMA. These results reveal a new degree of freedom to control PMA, enabling discovery of emergent magnetic textures and topological phenomena.