Voltage-Driven Fluorine Motion for Novel Organic Spintronic Memristor.

Integrating tunneling magnetoresistance (TMR) effect in memristors is a long-term aspiration because it allows to realize multifunctional devices, such as multi-state memory and tunable plasticity for synaptic function. However, the reported TMR in different multiferroic tunnel junctions is limited to 100%. This work demonstrates a giant TMR of -266% in La0.6Sr0.4MnO3(LSMO)/poly(vinylidene fluoride)(PVDF)/Co memristor with thin organic barrier. Different from the ferroelectricity-based memristors, this work discovers that the voltage-driven florine (F) motion in the junction generates a huge reversible resistivity change up to 106% with nanosecond (ns) timescale. Removing F from PVDF layer suppresses the dipole field in the tunneling barrier, thereby significantly enhances the TMR. Furthermore, the TMR can be tuned by different polarizing voltage due to the strong modification of spin-polarization at the LSMO/PVDF interface upon F doping. Combining of high TMR in the organic memristor paves the way to develop high-performance multifunctional devices for storage and neuromorphic applications.

Electrostatically controlled spin polarization in Graphene-CrSBr magnetic proximity heterostructures.

The magnetic proximity effect can induce a spin dependent exchange shift in the band structure of graphene. This produces a magnetization and a spin polarization of the electron/hole carriers in this material, paving the way for its use as an active component in spintronics devices. The electrostatic control of this spin polarization in graphene has however never been demonstrated so far. We show that interfacing graphene with the van der Waals antiferromagnet CrSBr results in an unconventional manifestation of the quantum Hall effect, which can be attributed to the presence of counterflowing spin-polarized edge channels originating from the spin-dependent exchange shift in graphene. We extract an exchange shift ranging from 27 - 32 meV, and show that it also produces an electrostatically tunable spin polarization of the electron/hole carriers in graphene ranging from - 50% to + 69% in the absence of a magnetic field. This proof of principle provides a starting point for the use of graphene as an electrostatically tunable source of spin current and could allow this system to generate a large magnetoresistance in gate tunable spin valve devices.

Atomic-Layer Controlled Transition from Inverse Rashba-Edelstein Effect to Inverse Spin Hall Effect in 2D PtSe2 Probed by THz Spintronic Emission.

2D materials, such as transition metal dichalcogenides, are ideal platforms for spin-to-charge conversion (SCC) as they possess strong spin-orbit coupling (SOC), reduced dimensionality and crystal symmetries as well as tuneable band structure, compared to metallic structures. Moreover, SCC can be tuned with the number of layers, electric field, or strain. Here, SCC in epitaxially grown 2D PtSe2 by THz spintronic emission is studied since its 1T crystal symmetry and strong SOC favor SCC. High quality of as-grown PtSe2 layers is demonstrated, followed by in situ ferromagnet deposition by sputtering that leaves the PtSe2 unaffected, resulting in well-defined clean interfaces as evidenced with extensive characterization. Through this atomic growth control and using THz spintronic emission, the unique thickness-dependent electronic structure of PtSe2 allows the control of SCC. Indeed, the transition from the inverse Rashba-Edelstein effect (IREE) in 1-3 monolayers (ML) to the inverse spin Hall effect (ISHE) in multilayers (>3 ML) of PtSe2 enabling the extraction of the perpendicular spin diffusion length and relative strength of IREE and ISHE is demonstrated. This band structure flexibility makes PtSe2 an ideal candidate to explore the underlying mechanisms and engineering of the SCC as well as for the development of tuneable THz spintronic emitters.

Artificial Graphene Spin Polarized Electrode for Magnetic Tunnel Junctions.

2D materials offer the ability to expose their electronic structure to manipulations by a proximity effect. This could be harnessed to craft properties of 2D interfaces and van der Waals heterostructures in devices and quantum materials. We explore the possibility to create an artificial spin polarized electrode from graphene through proximity interaction with a ferromagnetic insulator to be used in a magnetic tunnel junction (MTJ). Ferromagnetic insulator/graphene artificial electrodes were fabricated and integrated in MTJs based on spin analyzers. Evidence of the emergence of spin polarization in proximitized graphene layers was observed through the occurrence of tunnel magnetoresistance. We deduced a spin dependent splitting of graphene's Dirac band structure (∼15 meV) induced by the proximity effect, potentially leading to full spin polarization and opening the way to gating. The extracted spin signals illustrate the potential of 2D quantum materials based on proximity effects to craft spintronics functionalities, from vertical MTJs memory cells to logic circuits.

Gradient-Induced Dzyaloshinskii-Moriya Interaction.

The Dzyaloshinskii-Moriya interaction (DMI) that arises in the magnetic systems with broken inversion symmetry plays an essential role in topological spintronics. Here, by means of atomistic spin calculations, we study an intriguing type of DMI (g-DMI) that emerges in the films with composition gradient. We show that both the strength and chirality of g-DMI can be controlled by the composition gradient even in the disordered system. The layer-resolved analysis of g-DMI unveils its additive nature inside the bulk layers and clarifies the linear thickness dependence of g-DMI observed in experiments. Furthermore, we demonstrate the g-DMI-induced chiral magnetic structures, such as spin spirals and skyrmions, and the g-DMI driven field-free spin-orbit torque (SOT) switching, both of which are crucial toward practical device application. These results elucidate the underlying mechanisms of g-DMI and open up a new way to engineer the topological magnetic textures.

From Binary to Ternary Transition-Metal Nitrides: A Boost toward Nitrogen Magneto-Ionics.

Magneto-ionics is an emerging actuation mechanism to control the magnetic properties of materials via voltage-driven ion motion. This effect largely relies on the strength and penetration of the induced electric field into the target material, the amount of generated ion transport pathways, and the ionic mobility inside the magnetic media. Optimizing all these factors in a simple way is a huge challenge, although highly desirable for technological applications. Here, we demonstrate that the introduction of suitable transition-metal elements to binary nitride compounds can drastically boost magneto-ionics. More specifically, we show that the attained magneto-ionic effects in CoN films (i.e., saturation magnetization, toggling speeds, and cyclability) can be drastically enhanced through 10% substitution of Co by Mn in the thin-film composition. Incorporation of Mn leads to transformation from nanocrystalline into amorphous-like structures, as well as from metallic to semiconducting behaviors, resulting in an increase of N-ion transport channels. Ab initio calculations reveal a lower energy barrier for CoMn-N compared to Co-N that provides a fundamental understanding of the crucial role of Mn addition in the voltage-driven magnetic effects. These results constitute an important step forward toward enhanced voltage control of magnetism via electric field-driven ion motion.

Two-dimensional materials prospects for non-volatile spintronic memories.

Non-volatile magnetic random-access memories (MRAMs), such as spin-transfer torque MRAM and next-generation spin-orbit torque MRAM, are emerging as key to enabling low-power technologies, which are expected to spread over large markets from embedded memories to the Internet of Things. Concurrently, the development and performances of devices based on two-dimensional van der Waals heterostructures bring ultracompact multilayer compounds with unprecedented material-engineering capabilities. Here we provide an overview of the current developments and challenges in regard to MRAM, and then outline the opportunities that can arise by incorporating two-dimensional material technologies. We highlight the fundamental properties of atomically smooth interfaces, the reduced material intermixing, the crystal symmetries and the proximity effects as the key drivers for possible disruptive improvements for MRAM at advanced technology nodes.

The Magnetic Genome of Two-Dimensional van der Waals Materials.

Magnetism in two-dimensional (2D) van der Waals (vdW) materials has recently emerged as one of the most promising areas in condensed matter research, with many exciting emerging properties and significant potential for applications ranging from topological magnonics to low-power spintronics, quantum computing, and optical communications. In the brief time after their discovery, 2D magnets have blossomed into a rich area for investigation, where fundamental concepts in magnetism are challenged by the behavior of spins that can develop at the single layer limit. However, much effort is still needed in multiple fronts before 2D magnets can be routinely used for practical implementations. In this comprehensive review, prominent authors with expertise in complementary fields of 2D magnetism (i.e., synthesis, device engineering, magneto-optics, imaging, transport, mechanics, spin excitations, and theory and simulations) have joined together to provide a genome of current knowledge and a guideline for future developments in 2D magnetic materials research.

Skyrmions-based logic gates in one single nanotrack completely reconstructed via chirality barrier.

Logic gates based on magnetic elements are promising candidates for logic-in-memory applications with non-volatile data retention, near-zero leakage and scalability. In such spin-based logic devices, however, the multi-strip structure and fewer functions are obstacles to improving integration and reducing energy consumption. Here we propose a skyrmions-based single-nanotrack logic family including AND, OR, NOT, NAND, NOR, XOR and XNOR that can be implemented and reconstructed by building and switching the Dzyaloshinskii-Moriya interaction (DMI) chirality barrier on a racetrack memory. Besides the pinning effect of the DMI chirality barrier on skyrmions, the annihilation, fusion and shunting of two skyrmions with opposite chirality are also achieved and demonstrated via local reversal of the DMI, which are necessary for the design of an engineer programmable logic nanotrack, transistor and complementary racetrack memory.

Rashba-Type Dzyaloshinskii-Moriya Interaction, Perpendicular Magnetic Anisotropy, and Skyrmion States at 2D Materials/Co Interfaces.

We report a significant Dzyaloshinskii-Moriya interaction (DMI) and perpendicular magnetic anisotropy (PMA) at interfaces comprising hexagonal boron nitride (h-BN) and Co. By comparing the behavior of these phenomena at graphene/Co and h-BN/Co interfaces, it is found that the DMI in the latter increases as a function of Co thickness and beyond three monolayers stabilizes with 1 order of magnitude larger values compared to those at graphene/Co, where the DMI shows opposite decreasing behavior. Meanwhile, the PMA for both systems shows similar trends with larger values for graphene/Co and no significant variations for all thickness ranges of Co. Furthermore, using micromagnetic simulations we demonstrate that such significant DMI and PMA values remaining stable over a large range of Co thickness give rise to the formation of skyrmions with small applied external fields. These findings open up further possibilities toward integrating two-dimensional (2D) materials in spin-orbitronics devices.

Magneto-Ionics in Single-Layer Transition Metal Nitrides.

Magneto-ionics allows for tunable control of magnetism by voltage-driven transport of ions, traditionally oxygen or lithium and, more recently, hydrogen, fluorine, or nitrogen. Here, magneto-ionic effects in single-layer iron nitride films are demonstrated, and their performance is evaluated at room temperature and compared with previously studied cobalt nitrides. Iron nitrides require increased activation energy and, under high bias, exhibit more modest rates of magneto-ionic motion than cobalt nitrides. Ab initio calculations reveal that, based on the atomic bonding strength, the critical field required to induce nitrogen-ion motion is higher in iron nitrides (≈6.6 V nm-1) than in cobalt nitrides (≈5.3 V nm-1). Nonetheless, under large bias (i.e., well above the magneto-ionic onset and, thus, when magneto-ionics is fully activated), iron nitride films exhibit enhanced coercivity and larger generated saturation magnetization, surpassing many of the features of cobalt nitrides. The microstructural effects responsible for these enhanced magneto-ionic effects are discussed. These results open up the potential integration of magneto-ionics in existing nitride semiconductor materials in view of advanced memory system architectures.

Current-Driven Domain Wall Dynamics in Ferrimagnetic Nickel-Doped Mn4N Films: Very Large Domain Wall Velocities and Reversal of Motion Direction across the Magnetic Compensation Point.

Spin-transfer torque (STT) and spin-orbit torque (SOT) are spintronic phenomena allowing magnetization manipulation using electrical currents. Beyond their fundamental interest, they allow developing new classes of magnetic memories and logic devices, in particular based on domain wall (DW) motion. In this work, we report the study of STT-driven DW motion in ferrimagnetic manganese nickel nitride (Mn4-xNixN) films, in which magnetization and angular momentum compensation can be obtained by the fine adjustment of the Ni content. Large domain wall velocities, approaching 3000 m/s, are measured for Ni compositions close to the angular momentum compensation point. The reversal of the DW motion direction, observed when the compensation composition is crossed, is related to the change of direction of the angular momentum with respect to that of the spin polarization. This is confirmed by the results of ab initio band structure calculations.

Voltage-driven motion of nitrogen ions: a new paradigm for magneto-ionics.

Magneto-ionics, understood as voltage-driven ion transport in magnetic materials, has largely relied on controlled migration of oxygen ions. Here, we demonstrate room-temperature voltage-driven nitrogen transport (i.e., nitrogen magneto-ionics) by electrolyte-gating of a CoN film. Nitrogen magneto-ionics in CoN is compared to oxygen magneto-ionics in Co3O4. Both materials are nanocrystalline (face-centered cubic structure) and show reversible voltage-driven ON-OFF ferromagnetism. In contrast to oxygen, nitrogen transport occurs uniformly creating a plane-wave-like migration front, without assistance of diffusion channels. Remarkably, nitrogen magneto-ionics requires lower threshold voltages and exhibits enhanced rates and cyclability. This is due to the lower activation energy for ion diffusion and the lower electronegativity of nitrogen compared to oxygen. These results may open new avenues in applications such as brain-inspired computing or iontronics in general.

Coherent Resonant Tunneling through Double Metallic Quantum Well States.

Study of resonant tunneling through multimetallic quantum well (QW) structure is not only important for the fundamental understanding of quantum transport but also for the great potential to generate advanced functionalities of spintronic devices. However, it remains challenging to engineer such a structure due to the short electron phase coherence length in metallic QW system. Here, we demonstrate the successful fabrication of double-QW structure in a single fully epitaxial magnetic tunnel junction (MTJ) heterostructure, where two Fe QW layers are sandwiched between three MgAlO x tunnel barriers. We show clear evidence of the coherent resonant tunneling through the discrete QW states in the two QWs. The coherent resonant tunneling condition is fulfilled only when the middle barrier between the two QWs is thin enough and available QW states are present simultaneously in both QWs under a certain bias. Compared to the single QW structure, the resonant tunneling in double-QW MTJ produces strong conductivity oscillations with much narrower peak width (about half) owing to the enhanced energy filtering effect. This study presents a comprehensive understanding of the resonant tunneling mechanism in MTJ with multiple QWs, which is essential for future development of new spintronic devices operating in the quantum tunneling regime.

Controlling Dzyaloshinskii-Moriya Interaction via Chirality Dependent Atomic-Layer Stacking, Insulator Capping and Electric Field.

Using first-principles calculations, we demonstrate several approaches to control Dzyaloshinskii-Moriya Interaction (DMI) in ultrathin films with perpendicular magnetic anisotropy. First, we find that DMI is significantly enhanced when the ferromagnetic (FM) layer is sandwiched between nonmagnetic (NM) layers inducing additive DMI in NM1/FM/NM2 structures. For instance, when two NM layers are chosen to induce DMI of opposite chirality in Co, e.g. NM1 representing Au, Ir, Al or Pb, and NM2 being Pt, the resulting DMI in NM1/Co/Pt trilayers is enhanced compared to Co/Pt bilayers. Moreover, DMI can be significantly enhanced further in case of using FM layer comprising Fe and Co layers. Namely, it is found that the DMI in Ir/Fe/Co/Pt structure can be enhanced by 80% compared to that of Co/Pt bilayers reaching a very large DMI amplitude of 5.59 meV/atom. Our second approach for enhancing DMI is to use oxide capping layer. We show that DMI is enhanced by 60% in Oxide/Co/Pt structures compared to Co/Pt bilayers. Moreover, we unveiled the DMI mechanism at Oxide/Co interface due to Rashba effect, which is different to Fert-Levy DMI at FM/NM interfaces. Finally, we demonstrate that DMI amplitude can be modulated using an electric field with an efficiency factor comparable to that of the electric field control of perpendicular magnetic anisotropy in transition metal/oxide interfaces. These approaches of DMI controlling pave the way for skyrmion and domain wall motion-based spintronic applications.

Quenching of Spin Polarization Switching in Organic Multiferroic Tunnel Junctions by Ferroelectric "Ailing-Channel" in Organic Barrier.

The ferroelectric control of spin-polarization at ferromagnet (FM)/ferroelectric organic (FE-Org) interface by electrically switching the ferroelectric polarization of the FE-Org has been recently realized in the organic multiferroic tunnel junctions (OMFTJs) and gained intensive interests for future multifunctional organic spintronic applications. Here, we report the evidence of ferroelectric "ailing-channel" in the organic barrier, which can effectively pin the ferroelectric domain, resulting in nonswitchable spin polarization at the FM/FE-Org interface. In particular, OMFTJs based on La0.6Sr0.4MnO3/P(VDF-TrFE) ( t)/Co/Au structures with different P(VDF-TrFE) thickness ( t) were fabricated. The combined advanced electron microscopy and spectroscopy studies clearly reveal that very limited Co diffusion exists in the P(VDF-TrFE) organic barrier when the Au/Co electrode is deposited around 80K. Pot-hole structures at the boundary between the P(VDF-TrFE) needle-like grains are evidenced to induce "ailing-channels" that hinder efficient ferroelectric polarization of the organic barrier and result in the quenching of the spin polarization switching at Co/P(VDF-TrFE) interface. Furthermore, the spin diffusion length in the negatively polarized P(VDF-TrFE) is measured to be about 7.2 nm at 20K. The evidence of the mechanism of ferroelectric "ailing-channels" is of essential importance to improve the performance of OMFTJ and master the key condition for an efficient ferroelectric control of the spin polarization of "spinterface".

Symmetry broken spin reorientation transition in epitaxial MgO/Fe/MgO layers with competing anisotropies.

The observation of perpendicular magnetic anisotropy (PMA) at MgO/Fe interfaces boosted the development of spintronic devices based on ultrathin ferromagnetic layers. Yet, magnetization reversal in the standard magnetic tunnel junctions (MTJs) with competing PMA and in-plane anisotropies remains unclear. Here we report on the field induced nonvolatile broken symmetry magnetization reorientation transition from the in-plane to the perpendicular (out of plane) state at temperatures below 50 K. The samples were 10 nm thick Fe in MgO/Fe(100)/MgO as stacking components of V/MgO/Fe/MgO/Fe/Co double barrier MTJs with an area of 20 × 20 µm2. Micromagnetic simulations with PMA and different second order anisotropies at the opposite Fe/MgO interfaces qualitatively reproduce the observed broken symmetry spin reorientation transition. Our findings open the possibilities to develop multistate epitaxial spintronics based on competing magnetic anisotropies.

Large-Voltage Tuning of Dzyaloshinskii-Moriya Interactions: A Route toward Dynamic Control of Skyrmion Chirality.

Electric control of magnetism is a prerequisite for efficient and low-power spintronic devices. More specifically, in heavy metal-ferromagnet-insulator heterostructures, voltage gating has been shown to locally and dynamically tune magnetic properties such as interface anisotropy and saturation magnetization. However, its effect on interfacial Dzyaloshinskii-Moriya Interaction (DMI), which is crucial for the stability of magnetic skyrmions, has been challenging to achieve and has not been reported yet for ultrathin films. Here, we demonstrate a 130% variation of DMI with electric field in Ta/FeCoB/TaO x trilayer through Brillouin Light Spectroscopy (BLS). Using polar magneto-optical Kerr-effect microscopy, we further show a monotonic variation of DMI and skyrmionic bubble size with electric field with an unprecedented efficiency. We anticipate through our observations that a sign reversal of DMI with an electric field is possible, leading to a chirality switch. This dynamic manipulation of DMI establishes an additional degree of control to engineer programmable skyrmion-based memory or logic devices.

Spin Hall and Spin Swapping Torques in Diffusive Ferromagnets.

A complete set of the generalized drift-diffusion equations for a coupled charge and spin dynamics in ferromagnets in the presence of extrinsic spin-orbit coupling is derived from the quantum kinetic approach, covering major transport phenomena, such as the spin and anomalous Hall effects, spin swapping, spin precession, and relaxation processes. We argue that the spin swapping effect in ferromagnets is enhanced due to spin polarization, while the overall spin texture induced by the interplay of spin-orbital and spin precession effects displays a complex spatial dependence that can be exploited to generate torques and nucleate or propagate domain walls in centrosymmetric geometries without the use of external polarizers, as opposed to the conventional understanding of spin-orbit mediated torques.

Significant Dzyaloshinskii-Moriya interaction at graphene-ferromagnet interfaces due to the Rashba effect.

The possibility of utilizing the rich spin-dependent properties of graphene has attracted much attention in the pursuit of spintronics advances. The promise of high-speed and low-energy-consumption devices motivates the search for layered structures that stabilize chiral spin textures such as topologically protected skyrmions. Here we demonstrate that chiral spin textures are induced at graphene/ferromagnetic metal interfaces. Graphene is a weak spin-orbit coupling material and is generally not expected to induce a sufficient Dzyaloshinskii-Moriya interaction to affect magnetic chirality. We demonstrate that indeed graphene does induce a type of Dzyaloshinskii-Moriya interaction due to the Rashba effect. First-principles calculations and experiments using spin-polarized electron microscopy show that this graphene-induced Dzyaloshinskii-Moriya interaction can have a similar magnitude to that at interfaces with heavy metals. This work paves a path towards two-dimensional-material-based spin-orbitronics.