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.

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.

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.

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.

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.

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.

Voltage control of ferrimagnetic order and voltage-assisted writing of ferrimagnetic spin textures.

Voltage control of magnetic order is desirable for spintronic device applications, but 180° magnetization switching is not straightforward because electric fields do not break time-reversal symmetry. Ferrimagnets are promising candidates for 180° switching owing to a multi-sublattice configuration with opposing magnetic moments of different magnitudes. In this study we used solid-state hydrogen gating to control the ferrimagnetic order in rare earth-transition metal thin films dynamically. Electric field-induced hydrogen loading/unloading in GdCo can shift the magnetic compensation temperature by more than 100 K, which enables control of the dominant magnetic sublattice. X-ray magnetic circular dichroism measurements and ab initio calculations indicate that the magnetization control originates from the weakening of antiferromagnetic exchange coupling that reduces the magnetization of Gd more than that of Co upon hydrogenation. We observed reversible, gate voltage-induced net magnetization switching and full 180° Néel vector reversal in the absence of external magnetic fields. Furthermore, we generated ferrimagnetic spin textures, such as chiral domain walls and skyrmions, in racetrack devices through hydrogen gating. With gating times as short as 50 µs and endurance of more than 10,000 cycles, our method provides a powerful means to tune ferrimagnetic spin textures and dynamics, with broad applicability in the rapidly emerging field of ferrimagnetic spintronics.

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.

Relativistic kinematics of a magnetic soliton.

A tenet of special relativity is that no particle can exceed the speed of light. In certain magnetic materials, the maximum magnon group velocity serves as an analogous relativistic limit for the speed of magnetic solitons. Here, we drive domain walls to this limit in a low-dissipation magnetic insulator using pure spin currents from the spin Hall effect. We achieve record current-driven velocities in excess of 4300 meters per second-within ~10% of the relativistic limit-and we observe key signatures of relativistic motion associated with Lorentz contraction, which leads to velocity saturation. The experimental results are well explained through analytical and atomistic modeling. These observations provide critical insight into the fundamental limits of the dynamics of magnetic solitons and establish a readily accessible experimental framework to study relativistic solitonic physics.

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.

Interfacial Dzyaloshinskii-Moriya interaction arising from rare-earth orbital magnetism in insulating magnetic oxides.

The Dzyaloshinskii-Moriya interaction (DMI) is responsible for exotic chiral and topological magnetic states such as spin spirals and skyrmions. DMI manifests at metallic ferromagnet/heavy-metal interfaces, owing to inversion symmetry breaking and spin-orbit coupling by a heavy metal such as Pt. Moreover, in centrosymmetric magnetic oxides interfaced by Pt, DMI-driven topological spin textures and fast current-driven dynamics have been reported, though the origin of this DMI is unclear. While in metallic systems, spin-orbit coupling arises from a proximate heavy metal, we show that in perpendicularly-magnetized iron garnets, rare-earth orbital magnetism gives rise to an intrinsic spin-orbit coupling generating interfacial DMI at mirror symmetry-breaking interfaces. We show that rare-earth ion substitution and strain engineering can significantly alter the DMI. These results provide critical insights into the origins of chiral magnetism in low-damping magnetic oxides and identify paths toward engineering chiral and topological states in centrosymmetric oxides through rare-earth ion substitution.

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.

Voltage-gated optics and plasmonics enabled by solid-state proton pumping.

Devices with locally-addressable and dynamically tunable optical properties underpin emerging technologies such as high-resolution reflective displays and dynamic holography. The optical properties of metals such as Y and Mg can be reversibly switched by hydrogen loading, and hydrogen-switched mirrors and plasmonic devices have been realized, but challenges remain to achieve electrical, localized and reversible control. Here we report a nanoscale solid-state proton switch that allows for electrical control of optical properties through electrochemical hydrogen gating. We demonstrate the generality and versatility of this approach by realizing tunability of a range of device characteristics including transmittance, interference color, and plasmonic resonance. We further discover and exploit a giant modulation of the effective refractive index of the gate dielectric. The simple gate structure permits device thickness down to ~20 nanometers, which can enable device scaling into the deep subwavelength regime, and has potential applications in addressable plasmonic devices and reconfigurable metamaterials.

Interface-driven chiral magnetism and current-driven domain walls in insulating magnetic garnets.

Magnetic oxides exhibit rich fundamental physics1-4 and technologically desirable properties for spin-based memory, logic and signal transmission5-7. Recently, spin-orbit-induced spin transport phenomena have been realized in insulating magnetic oxides by using proximate heavy metal layers such as platinum8-10. In their metallic ferromagnet counterparts, such interfaces also give rise to a Dzyaloshinskii-Moriya interaction11-13 that can stabilize homochiral domain walls and skyrmions with efficient current-driven dynamics. However, chiral magnetism in centrosymmetric oxides has not yet been observed. Here we discover chiral magnetism that allows for pure spin-current-driven domain wall motion in the most ubiquitous class of magnetic oxides, ferrimagnetic iron garnets. We show that epitaxial rare-earth iron garnet films with perpendicular magnetic anisotropy exhibit homochiral Néel domain walls that can be propelled faster than 800 m s-1 by spin current from an adjacent platinum layer. We find that, despite the relatively small interfacial Dzyaloshinskii-Moriya interaction, very high velocities can be attained due to the antiferromagnetic spin dynamics associated with ferrimagnetic order.

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.

Current-Induced Skyrmion Generation through Morphological Thermal Transitions in Chiral Ferromagnetic Heterostructures.

Magnetic skyrmions promise breakthroughs in future memory and computing devices due to their inherent stability and small size. Their creation and current driven motion have been recently observed at room temperature, but the key mechanisms of their formation are not yet well-understood. Here it is shown that in heavy metal/ferromagnet heterostructures, pulsed currents can drive morphological transitions between labyrinth-like, stripe-like, and skyrmionic states. Using high-resolution X-ray microscopy, the spin texture evolution with temperature and magnetic field is imaged and it is demonstrated that with transient Joule heating, topological charges can be injected into the system, driving it across the stripe-skyrmion boundary. The observations are explained through atomistic spin dynamic and micromagnetic simulations that reveal a crossover to a global skyrmionic ground state above a threshold magnetic field, which is found to decrease with increasing temperature. It is demonstrated how by tuning the phase stability, one can reliably generate skyrmions by short current pulses and stabilize them at zero field, providing new means to create and manipulate spin textures in engineered chiral ferromagnets.

Fast current-driven domain walls and small skyrmions in a compensated ferrimagnet.

Spintronics is a research field that aims to understand and control spins on the nanoscale and should enable next-generation data storage and manipulation. One technological and scientific key challenge is to stabilize small spin textures and to move them efficiently with high velocities. For a long time, research focused on ferromagnetic materials, but ferromagnets show fundamental limits for speed and size. Here, we circumvent these limits using compensated ferrimagnets. Using ferrimagnetic Pt/Gd44Co56/TaOx films with a sizeable Dzyaloshinskii-Moriya interaction, we realize a current-driven domain wall motion with a speed of 1.3 km s-1 near the angular momentum compensation temperature (TA) and room-temperature-stable skyrmions with minimum diameters close to 10 nm near the magnetic compensation temperature (TM). Both the size and dynamics of the ferrimagnet are in excellent agreement with a simplified effective ferromagnet theory. Our work shows that high-speed, high-density spintronics devices based on current-driven spin textures can be realized using materials in which TA and TM are close together.

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.