Coherent correlation imaging for resolving fluctuating states of matter.

Fluctuations and stochastic transitions are ubiquitous in nanometre-scale systems, especially in the presence of disorder. However, their direct observation has so far been impeded by a seemingly fundamental, signal-limited compromise between spatial and temporal resolution. Here we develop coherent correlation imaging (CCI) to overcome this dilemma. Our method begins by classifying recorded camera frames in Fourier space. Contrast and spatial resolution emerge by averaging selectively over same-state frames. Temporal resolution down to the acquisition time of a single frame arises independently from an exceptionally low misclassification rate, which we achieve by combining a correlation-based similarity metric1,2 with a modified, iterative hierarchical clustering algorithm3,4. We apply CCI to study previously inaccessible magnetic fluctuations in a highly degenerate magnetic stripe domain state with nanometre-scale resolution. We uncover an intricate network of transitions between more than 30 discrete states. Our spatiotemporal data enable us to reconstruct the pinning energy landscape and to thereby explain the dynamics observed on a microscopic level. CCI massively expands the potential of emerging high-coherence X-ray sources and paves the way for addressing large fundamental questions such as the contribution of pinning5-8 and topology9-12 in phase transitions and the role of spin and charge order fluctuations in high-temperature superconductivity13,14.

Temperature-Dependent Surface Anisotropy in (110) Epitaxial Rare Earth Iron Garnet Films.

Ferrimagnetic oxide thin films are important material platforms for spintronic devices. Films grown on low symmetry orientations such as (110) exhibit complex anisotropy landscapes that can provide insight into novel phenomena such as spin-torque auto-oscillation and spin superfluidity. Using spin-Hall magnetoresistance measurements, the in-plane (IP) and out-of-plane (OOP) uniaxial anisotropy energies are determined for a thickness series (5-50 nm) of europium iron garnet (EuIG) and thulium iron garnet (TmIG) films epitaxially grown on a gadolinium gallium substrate with (110) orientation and capped with Pt. Pt/EuIG/GGG exhibits an (001) easy plane of magnetization perpendicular to the substrate, whereas Pt/TmIG/GGG exhibits an (001) hard plane of magnetization perpendicular to the substrate with an IP easy axis. Both IP and OOP surface anisotropy energies comparable in magnitude to the bulk anisotropy are observed. The temperature dependence of the surface anisotropies is consistent with first-order predictions of a simplified Néel surface anisotropy model. By taking advantage of the thickness and temperature dependence demonstrated in these ferrimagnetic oxides grown on the low symmetry (110) orientations, the complex anisotropy landscapes can be tuned to act as a platform to explore rich spin textures and dynamics.

Ferrimagnetic spintronics.

Ferrimagnets composed of multiple and antiferromagnetically coupled magnetic elements have attracted much attention recently as a material platform for spintronics. They offer the combined advantages of both ferromagnets and antiferromagnets, namely the easy control and detection of their net magnetization by an external field, antiferromagnetic-like dynamics faster than ferromagnetic dynamics and the potential for high-density devices. This Review summarizes recent progress in ferrimagnetic spintronics, with particular attention to the most-promising functionalities of ferrimagnets, which include their spin transport, spin texture dynamics and all-optical switching.

Erratum: Large Anomalous Frequency Shift in Perpendicular Standing Spin Wave Modes in BiYIG Films Induced by Thin Metallic Overlayers [Phys. Rev. Lett. 130, 126703 (2023)].

This corrects the article DOI: 10.1103/PhysRevLett.130.126703.

Large Anomalous Frequency Shift in Perpendicular Standing Spin Wave Modes in BiYIG Films Induced by Thin Metallic Overlayers.

Interface-driven effects on magnon dynamics are studied in magnetic insulator-metal bilayers using Brillouin light scattering. It is found that the Damon-Eshbach modes exhibit a significant frequency shift due to interfacial anisotropy generated by thin metallic overlayers. In addition, an unexpectedly large shift in the perpendicular standing spin wave mode frequencies is also observed, which cannot be explained by anisotropy-induced mode stiffening or surface pinning. Rather, it is suggested that additional confinement may result from spin pumping at the insulator-metal interface, which results in a locally overdamped interface region. These results uncover previously unidentified interface-driven changes in magnetization dynamics that may be exploited to locally control and modulate magnonic properties in thin-film heterostructures.

Observation of fluctuation-mediated picosecond nucleation of a topological phase.

Topological states of matter exhibit fascinating physics combined with an intrinsic stability. A key challenge is the fast creation of topological phases, which requires massive reorientation of charge or spin degrees of freedom. Here we report the picosecond emergence of an extended topological phase that comprises many magnetic skyrmions. The nucleation of this phase, followed in real time via single-shot soft X-ray scattering after infrared laser excitation, is mediated by a transient topological fluctuation state. This state is enabled by the presence of a time-reversal symmetry-breaking perpendicular magnetic field and exists for less than 300 ps. Atomistic simulations indicate that the fluctuation state largely reduces the topological energy barrier and thereby enables the observed rapid and homogeneous nucleation of the skyrmion phase. These observations provide fundamental insights into the nature of topological phase transitions, and suggest a path towards ultrafast topological switching in a wide variety of materials through intermediate fluctuating states.

Fast Magneto-Ionic Switching of Interface Anisotropy Using Yttria-Stabilized Zirconia Gate Oxide.

Voltage control of interfacial magnetism has been greatly highlighted in spintronics research for many years, as it might enable ultralow power technologies. Among a few suggested approaches, magneto-ionic control of magnetism has demonstrated large modulation of magnetic anisotropy. Moreover, the recent demonstration of magneto-ionic devices using hydrogen ions presented relatively fast magnetization toggle switching, tsw ∼ 100 ms, at room temperature. However, the operation speed may need to be significantly improved to be used for modern electronic devices. Here, we demonstrate that the speed of proton-induced magnetization toggle switching largely depends on proton-conducting oxides. We achieve ∼1 ms reliable (>103 cycles) switching using yttria-stabilized zirconia (YSZ), which is ∼100 times faster than the state-of-the-art magneto-ionic devices reported to date at room temperature. Our results suggest that further engineering of the proton-conducting materials could bring substantial improvement that may enable new low-power computing scheme based on magneto-ionics.

Magneto-ionic control of magnetism using a solid-state proton pump.

Voltage-gated ion transport as a means of manipulating magnetism electrically could enable ultralow-power memory, logic and sensor technologies. Earlier work made use of electric-field-driven O2- displacement to modulate magnetism in thin films by controlling interfacial or bulk oxidation states. However, elevated temperatures are required and chemical and structural changes lead to irreversibility and device degradation. Here we show reversible and non-destructive toggling of magnetic anisotropy at room temperature using a small gate voltage through H+ pumping in all-solid-state heterostructures. We achieve 90° magnetization switching by H+ insertion at a Co/GdOx interface, with no degradation in magnetic properties after >2,000 cycles. We then demonstrate reversible anisotropy gating by hydrogen loading in Pd/Co/Pd heterostructures, making metal-metal interfaces susceptible to voltage control. The hydrogen storage metals Pd and Pt are high spin-orbit coupling materials commonly used to generate perpendicular magnetic anisotropy, Dzyaloshinskii-Moriya interaction, and spin-orbit torques in ferromagnet/heavy-metal heterostructures. Thus, our work provides a platform for voltage-controlled spin-orbitronics.

Nonlocal Detection of Out-of-Plane Magnetization in a Magnetic Insulator by Thermal Spin Drag.

We demonstrate a conceptually new mechanism to generate an in-plane spin current with out-of-plane polarization in a nonmagnetic metal, detected by nonlocal thermoelectric voltage measurement. We generate out-of-plane (∇T_{OP}) and in-plane (∇T_{IP}) temperature gradients, simultaneously, acting on a magnetic insulator-Pt bilayer. When the magnetization has a component oriented perpendicular to the plane, ∇T_{OP} drives a spin current into Pt with out-of-plane polarization due to the spin Seebeck effect. ∇T_{IP} then drags the resulting spin-polarized electrons in Pt parallel to the plane against the gradient direction. This finally produces an inverse spin Hall effect voltage in Pt, transverse to ∇T_{IP} and proportional to the out-of-plane component of the magnetization. This simple method enables the detection of the perpendicular magnetization component in a magnetic insulator in a nonlocal geometry.

Current-induced switching in a magnetic insulator.

The spin Hall effect in heavy metals converts charge current into pure spin current, which can be injected into an adjacent ferromagnet to exert a torque. This spin-orbit torque (SOT) has been widely used to manipulate the magnetization in metallic ferromagnets. In the case of magnetic insulators (MIs), although charge currents cannot flow, spin currents can propagate, but current-induced control of the magnetization in a MI has so far remained elusive. Here we demonstrate spin-current-induced switching of a perpendicularly magnetized thulium iron garnet film driven by charge current in a Pt overlayer. We estimate a relatively large spin-mixing conductance and damping-like SOT through spin Hall magnetoresistance and harmonic Hall measurements, respectively, indicating considerable spin transparency at the Pt/MI interface. We show that spin currents injected across this interface lead to deterministic magnetization reversal at low current densities, paving the road towards ultralow-dissipation spintronic devices based on MIs.

Origins of the Unidirectional Spin Hall Magnetoresistance in Metallic Bilayers.

Recent studies evidenced the emergence of asymmetric electron transport in layered conductors owing to the interplay between electrical conductivity, magnetization, and the spin Hall or Rashba-Edelstein effects. Here, we investigate the unidirectional magnetoresistance (UMR) caused by the current-induced spin accumulation in Co/Pt and CoCr/Pt bilayers. We identify three competing mechanisms underpinning the resistance asymmetry, namely, interface and bulk spin-dependent electron scattering and electron-magnon scattering. Our measurements provide a consistent description of the current, magnetic field, and temperature dependence of the UMR and show that both positive and negative UMR can be obtained by tuning the interface and bulk spin-dependent scattering.

Observation of room-temperature magnetic skyrmions and their current-driven dynamics in ultrathin metallic ferromagnets.

Magnetic skyrmions are topologically protected spin textures that exhibit fascinating physical behaviours and large potential in highly energy-efficient spintronic device applications. The main obstacles so far are that skyrmions have been observed in only a few exotic materials and at low temperatures, and fast current-driven motion of individual skyrmions has not yet been achieved. Here, we report the observation of stable magnetic skyrmions at room temperature in ultrathin transition metal ferromagnets with magnetic transmission soft X-ray microscopy. We demonstrate the ability to generate stable skyrmion lattices and drive trains of individual skyrmions by short current pulses along a magnetic racetrack at speeds exceeding 100 m s(-1) as required for applications. Our findings provide experimental evidence of recent predictions and open the door to room-temperature skyrmion spintronics in robust thin-film heterostructures.

Magneto-ionic control of interfacial magnetism.

In metal/oxide heterostructures, rich chemical, electronic, magnetic and mechanical properties can emerge from interfacial chemistry and structure. The possibility to dynamically control interface characteristics with an electric field paves the way towards voltage control of these properties in solid-state devices. Here, we show that electrical switching of the interfacial oxidation state allows for voltage control of magnetic properties to an extent never before achieved through conventional magneto-electric coupling mechanisms. We directly observe in situ voltage-driven O(2-) migration in a Co/metal-oxide bilayer, which we use to toggle the interfacial magnetic anisotropy energy by >0.75 erg cm(-2) at just 2 V. We exploit the thermally activated nature of ion migration to markedly increase the switching efficiency and to demonstrate reversible patterning of magnetic properties through local activation of ionic migration. These results suggest a path towards voltage-programmable materials based on solid-state switching of interface oxygen chemistry.

Current-driven dynamics of chiral ferromagnetic domain walls.

In most ferromagnets the magnetization rotates from one domain to the next with no preferred handedness. However, broken inversion symmetry can lift the chiral degeneracy, leading to topologically rich spin textures such as spin spirals and skyrmions through the Dzyaloshinskii-Moriya interaction (DMI). Here we show that in ultrathin metallic ferromagnets sandwiched between a heavy metal and an oxide, the DMI stabilizes chiral domain walls (DWs) whose spin texture enables extremely efficient current-driven motion. We show that spin torque from the spin Hall effect drives DWs in opposite directions in Pt/CoFe/MgO and Ta/CoFe/MgO, which can be explained only if the DWs assume a Néel configuration with left-handed chirality. We directly confirm the DW chirality and rigidity by examining current-driven DW dynamics with magnetic fields applied perpendicular and parallel to the spin spiral. This work resolves the origin of controversial experimental results and highlights a new path towards interfacial design of spintronic devices.

Damping and Interfacial Dzyaloshinskii-Moriya Interaction in Thulium Iron Garnet/Bismuth-Substituted Yttrium Iron Garnet Bilayers.

Thin films of ferrimagnetic iron garnets can exhibit useful magnetic properties, including perpendicular magnetic anisotropy (PMA) and high domain wall velocities. In particular, bismuth-substituted yttrium iron garnet (BiYIG) films grown on garnet substrates have a low Gilbert damping but zero Dzyaloshinskii-Moriya interaction (DMI), whereas thulium iron garnet (TmIG) films have higher damping but a nonzero DMI. We report the damping and DMI of thulium-substituted BiYIG (BiYTmIG) and TmIG|BiYIG bilayer thin films deposited on (111) substituted gadolinium gallium garnet and neodymium gallium garnet (NGG) substrates. The films are epitaxial and exhibit PMA. BiYIG|TmIG bilayers have a damping value that is an order of magnitude lower than that of TmIG, and BiYIG|TmIG|NGG have DMI of 0.0145 ± 0.0011 mJ/m2, similar to that of TmIG|NGG. The bilayer therefore provides a combination of DMI and moderate damping, useful for the development of high-speed spin orbit torque-driven devices.

Atomic order of rare earth ions in a complex oxide: a path to magnetotaxial anisotropy.

Complex oxides offer rich magnetic and electronic behavior intimately tied to the composition and arrangement of cations within the structure. Rare earth iron garnet films exhibit an anisotropy along the growth direction which has long been theorized to originate from the ordering of different cations on the same crystallographic site. Here, we directly demonstrate the three-dimensional ordering of rare earth ions in pulsed laser deposited (EuxTm1-x)3Fe5O12 garnet thin films using both atomically-resolved elemental mapping to visualize cation ordering and X-ray diffraction to detect the resulting order superlattice reflection. We quantify the resulting ordering-induced 'magnetotaxial' anisotropy as a function of Eu:Tm ratio using transport measurements, showing an overwhelmingly dominant contribution from magnetotaxial anisotropy that reaches 30 kJ m-3 for garnets with x = 0.5. Control of cation ordering on inequivalent sites provides a strategy to control matter on the atomic level and to engineer the magnetic properties of complex oxides.

Magnetoelectric charge trap memory.

It is demonstrated that a charge-trapping layer placed in proximity to a ferromagnetic metal enables efficient electrical and optical control of the metal's magnetic properties. Retention of charge trapped inside the charge-trapping layer provides nonvolatility to the magnetoelectric effect and enhances its efficiency by an order of magnitude. As such, an engineered charge-trapping layer can be used to realize the magnetoelectric equivalent to today's pervasive charge trap flash memory technology. Moreover, by supplying trapped charges optically instead of electrically, a focused laser beam can be used to imprint the magnetic state into a continuous metal film.

Large exchange bias enhancement and control of ferromagnetic energy landscape by solid-state hydrogen gating.

Voltage control of exchange bias is desirable for spintronic device applications, however dynamic modulation of the unidirectional coupling energy in ferromagnet/antiferromagnet bilayers has not yet been achieved. Here we show that by solid-state hydrogen gating, perpendicular exchange bias can be enhanced by > 100% in a reversible and analog manner, in a simple Co/Co0.8Ni0.2O heterostructure at room temperature. We show that this phenomenon is an isothermal analog to conventional field-cooling and that sizable changes in average coupling energy can result from small changes in AFM grain rotatability. Using this method, we show that a bi-directionally stable ferromagnet can be made unidirectionally stable, with gate voltage alone. This work provides a means to dynamically reprogram exchange bias, with broad applicability in spintronics and neuromorphic computing, while simultaneously illuminating fundamental aspects of exchange bias in polycrystalline films.

Voltage control of magnetic order in RKKY coupled multilayers.

In the field of antiferromagnetic (AFM) spintronics, there is a substantial effort present to make AFMs viable active components for efficient and fast devices. Typically, this is done by manipulating the AFM Néel vector. Here, we establish a method of enabling AFM active components by directly controlling the magnetic order. We show that magneto-ionic gating of hydrogen enables dynamic control of the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction in solid-state synthetic AFM multilayer devices. Using a gate voltage, we tune the RKKY interaction to drive continuous transitions from AFM to FM and vice versa. The switching is submillisecond at room temperature and fully reversible. We validate the utility of this method by demonstrating that magneto-ionic gating of the RKKY interaction allows for 180° field-free deterministic switching. This dynamic method of controlling a fundamental exchange interaction can engender the manipulation of a broader array of spin textures, e.g., chiral domain walls and skyrmions.