Spatially reconfigurable antiferromagnetic states in topologically rich free-standing nanomembranes.

Antiferromagnets hosting real-space topological textures are promising platforms to model fundamental ultrafast phenomena and explore spintronics. However, they have only been epitaxially fabricated on specific symmetry-matched substrates, thereby preserving their intrinsic magneto-crystalline order. This curtails their integration with dissimilar supports, restricting the scope of fundamental and applied investigations. Here we circumvent this limitation by designing detachable crystalline antiferromagnetic nanomembranes of α-Fe2O3. First, we show-via transmission-based antiferromagnetic vector mapping-that flat nanomembranes host a spin-reorientation transition and rich topological phenomenology. Second, we exploit their extreme flexibility to demonstrate the reconfiguration of antiferromagnetic states across three-dimensional membrane folds resulting from flexure-induced strains. Finally, we combine these developments using a controlled manipulator to realize the strain-driven non-thermal generation of topological textures at room temperature. The integration of such free-standing antiferromagnetic layers with flat/curved nanostructures could enable spin texture designs via magnetoelastic/geometric effects in the quasi-static and dynamical regimes, opening new explorations into curvilinear antiferromagnetism and unconventional computing.

Tunable Spin-Polarized States in Graphene on a Ferrimagnetic Oxide Insulator.

Spin-polarized two-dimensional (2D) materials with large and tunable spin-splitting energy promise the field of 2D spintronics. While graphene has been a canonical 2D material, its spin properties and tunability are limited. Here, this work demonstrates the emergence of robust spin-polarization in graphene with large and tunable spin-splitting energy of up to 132 meV at zero applied magnetic fields. The spin polarization is induced through a magnetic exchange interaction between graphene and the underlying ferrimagnetic oxide insulating layer, Tm3 Fe5 O12 , as confirmed by its X-ray magnetic circular dichroism (XMCD). The spin-splitting energies are directly measured and visualized by the shift in their Landau-fan diagram mapped by analyzing the measured Shubnikov-de-Haas (SdH) oscillations as a function of applied electric fields, showing consistent fit with the first-principles and machine learning calculations. Further, the observed spin-splitting energies can be tuned over a broad range between 98 and 166 meV by field cooling. The methods and results are applicable to other 2D (magnetic) materials and heterostructures, and offer great potential for developing next-generation spin logic and memory devices.

Tunable Magnetic Properties in Sr2FeReO6 Double-Perovskite.

Double-perovskite oxides have attracted recent attention due to their attractive functionalities and application potential. In this paper, we demonstrate the effect of dual controls, i.e., the deposition pressure of oxygen (PO2) and lattice mismatch (ε), on tuning magnetic properties in epitaxial double-perovskite Sr2FeReO6 films. In a nearly lattice matched Sr2FeReO6/SrTiO3 film, the ferrimagnetic-to-paramagnetic phase transition occurs when PO2 is reduced to 30 mTorr, probably due to the formation of Re4+ ions that replace the stoichiometric Re5+ to cause disorders of B-site ions. On the other hand, a large compressive strain or tensile strain shifts this critical PO2 to below 1 mTorr or above 40 mTorr, respectively. The observations can be attributed to the modulation of B-site ordering by epitaxial strain through affecting elemental valence. Our results provide a feasible way to expand the functional tunability of magnetic double-perovskite oxides that hold great promise for spintronic devices.

Reversible hydrogen control of antiferromagnetic anisotropy in α-Fe2O3.

Antiferromagnetic insulators are a ubiquitous class of magnetic materials, holding the promise of low-dissipation spin-based computing devices that can display ultra-fast switching and are robust against stray fields. However, their imperviousness to magnetic fields also makes them difficult to control in a reversible and scalable manner. Here we demonstrate a novel proof-of-principle ionic approach to control the spin reorientation (Morin) transition reversibly in the common antiferromagnetic insulator α-Fe2O3 (haematite) - now an emerging spintronic material that hosts topological antiferromagnetic spin-textures and long magnon-diffusion lengths. We use a low-temperature catalytic-spillover process involving the post-growth incorporation or removal of hydrogen from α-Fe2O3 thin films. Hydrogenation drives pronounced changes in its magnetic anisotropy, Néel vector orientation and canted magnetism via electron injection and local distortions. We explain these effects with a detailed magnetic anisotropy model and first-principles calculations. Tailoring our work for future applications, we demonstrate reversible control of the room-temperature spin-state by doping/expelling hydrogen in Rh-substituted α-Fe2O3.

Emergent Topological Hall Effect at a Charge-Transfer Interface.

Exploring exotic interface magnetism due to charge transfer and strong spin-orbit coupling has profound application in the future development of spintronic memory. Here, the emergence and tuning of topological Hall effect (THE) from a CaMnO3 /CaIrO3 /CaMnO3 trilayer structure are studied in detail, which suggests the presence of magnetic Skyrmion-like bubbles. First, by tilting the magnetic field direction, the evolution of the Hall signal suggests a transformation of Skyrmions into topologically-trivial stripe domains, consistent with behaviors predicted by micromagnetic simulations. Second, by varying the thickness of CaMnO3 , the optimal thicknesses for the THE signal emergence are found, which allow identification of the source of Dzyaloshinskii-Moriya interaction (DMI) and its competition with antiferromagnetic superexchange. Employing high-resolution transmission electron microscopy, randomly distributed stacking faults are identified only at the bottom interface and may avoid mutual cancellation of DMI. Last, a spin-transfer torque experiment also reveals a low threshold current density of ≈109 A m-2 for initiating the bubbles' motion. This discovery sheds light on a possible strategy for integrating Skyrmions with antiferromagnetic spintronics.

Phase Diagram and Superconducting Dome of Infinite-Layer Nd_{1-x}Sr_{x}NiO_{2} Thin Films.

Infinite-layer Nd_{1-x}Sr_{x}NiO_{2} thin films with Sr doping level x from 0.08 to 0.3 are synthesized and investigated. We find a superconducting dome x between 0.12 and 0.235 accompanied by a weakly insulating behavior in both under- and overdoped regimes. The dome is akin to that in the electron-doped 214-type and infinite-layer cuprate superconductors. For x≥0.18, the normal state Hall coefficient (R_{H}) changes the sign from negative to positive as the temperature decreases. The temperature of the sign changes decreases monotonically with decreasing x from the overdoped side and approaches the superconducting dome at the midpoint, suggesting a reconstruction of the Fermi surface with the dopant concentration across the dome.

Room-Temperature Colossal Magnetoresistance in Terraced Single-Layer Graphene.

Disorder-induced magnetoresistance (MR) effect is quadratic at low perpendicular magnetic fields and linear at high fields. This effect is technologically appealing, especially in 2D materials such as graphene, since it offers potential applications in magnetic sensors with nanoscale spatial resolution. However, it is a great challenge to realize a graphene magnetic sensor based on this effect because of the difficulty in controlling the spatial distribution of disorder and enhancing the MR sensitivity in the single-layer regime. Here, a room-temperature colossal MR of up to 5000% at 9 T is reported in terraced single-layer graphene. By laminating single-layer graphene on a terraced substrate, such as TiO2 -terminated SrTiO3 , a universal one order of magnitude enhancement in the MR compared to conventional single-layer graphene devices is demonstrated. Strikingly, a colossal MR of >1000% is also achieved in the terraced graphene even at a high carrier density of ≈1012 cm-2 . Systematic studies of the MR of single-layer graphene on various oxide- and non-oxide-based terraced surfaces demonstrate that the terraced structure is the dominant factor driving the MR enhancement. The results open a new route for tailoring the physical property of 2D materials by engineering the strain through a terraced substrate.

Characteristic Lengths of Interlayer Charge Transfer in Correlated Oxide Heterostructures.

Using interlayer interaction to control functional heterostructures with atomic-scale designs has become one of the most effective interface-engineering strategies nowadays. Here, we demonstrate the effect of a crystalline LaFeO3 buffer layer on amorphous and crystalline LaAlO3/SrTiO3 heterostructures. The LaFeO3 buffer layer acts as an energetically favored electron acceptor in both LaAlO3/SrTiO3 systems, resulting in modulation of interfacial carrier density and hence metal-to-insulator transition. For amorphous and crystalline LaAlO3/SrTiO3 heterostructures, the metal-to-insulator transition is found when the LaFeO3 layer thickness crosses 3 and 6 unit cells, respectively. Such different critical LaFeO3 thicknesses are explained in terms of distinct characteristic lengths of the redox-reaction-mediated and polar-catastrophe-dominated charge transfer, controlled by the interfacial atomic contact and Thomas-Fermi screening effect, respectively. Our results not only shed light on the complex interlayer charge transfer across oxide heterostructures but also provide a new route to precisely tailor the charge-transfer process at a functional interface.

Magnetic Anisotropy of a Quasi Two-Dimensional Canted Antiferromagnet.

We report the control of the interplane magnetic exchange coupling in CaIrO3 perovskite thin films and superlattices with SrTiO3. By analyzing the anisotropic magneto-transport data, we demonstrate that a semimetallic paramagnetic CaIrO3 turns into a canted antiferromagnetic Mott insulator at reduced dimensions. The emergence of a biaxial magneto-crystalline anisotropy indicates the canted moment responding to the cubic symmetry. Extending to superlattices and probing oxygen octahedral rotation by half-integer X-ray Braggs diffraction, a more complete picture about the canted moment evolution with interplane coupling can be understood. Remarkably, a rotation of the canted moments' easy axes by 45° is also observed by a sign reversal of the in-plane strain. These results demonstrate the robustness of anisotropic magnetoresistance in revealing quasi two-dimensional canted antiferromagnets, as well as valuable insights about quadrupolar magnetoelastic coupling, relevant for designing future antiferromagnetic spintronic devices.