Field-Free Switching of Perpendicular Magnetization in an Ultrathin Epitaxial Magnetic Insulator.

For energy-efficient magnetic memories, switching of perpendicular magnetization by spin-orbit torque (SOT) appears to be a promising solution. This SOT switching requires the assistance of an in-plane magnetic field to break the symmetry. Here, we demonstrate the field-free SOT switching of a perpendicularly magnetized thulium iron garnet (Tm3Fe5O12, TmIG). The polarity of the switching loops, clockwise or counterclockwise, is determined by the direction of the initial current pulses, in contrast with field-assisted switching where the polarity is controlled by the direction of the magnetic field. From Brillouin light scattering, we determined the Dzyaloshinskii-Moriya interaction (DMI) induced by the Pt-TmIG interface. We will discuss the possible origins of field-free switching and the roles of the interfacial DMI and cubic magnetic anisotropy of TmIG. This discussion is substantiated by magnetotransport, Kerr microscopy, and micromagnetic simulations. Our observation of field-free electrical switching of a magnetic insulator is an important milestone for low-power spintronic devices.

Onset of Multiferroicity in Prototypical Single-Spin Cycloid BiFeO3 Thin Films.

In the room-temperature magnetoelectric multiferroic BiFeO3, the noncollinear antiferromagnetic state is coupled to the ferroelectric order, opening applications for low-power electric-field-controlled magnetic devices. While several strategies have been explored to simplify the ferroelectric landscape, here we directly stabilize a single-domain ferroelectric and spin cycloid state in epitaxial BiFeO3 (111) thin films grown on orthorhombic DyScO3 (011). Comparing them with films grown on SrTiO3 (111), we identify anisotropic in-plane strain as a powerful handle for tailoring the single antiferromagnetic state. In this single-domain multiferroic state, we establish the thickness limit of the coexisting electric and magnetic orders and directly visualize the suppression of the spin cycloid induced by the magnetoelectric interaction below the ultrathin limit of 1.4 nm. This as-grown single-domain multiferroic configuration in BiFeO3 thin films opens an avenue both for fundamental investigations and for electrically controlled noncollinear antiferromagnetic spintronics.

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.

Three-dimensional skyrmionic cocoons in magnetic multilayers.

Three-dimensional spin textures emerge as promising quasi-particles for encoding information in future spintronic devices. The third dimension provides more malleability regarding their properties and more flexibility for potential applications. However, the stabilization and characterization of such quasi-particles in easily implementable systems remain a work in progress. Here we observe a three-dimensional magnetic texture that sits in the interior of magnetic thin films aperiodic multilayers and possesses a characteristic ellipsoidal shape. Interestingly, these objects that we call skyrmionic cocoons can coexist with more standard tubular skyrmions going through all the multilayer as evidenced by the existence of two very different contrasts in room temperature magnetic force microscopy. The presence of these novel skyrmionic textures as well as the understanding of their layer resolved chiral and topological properties have been investigated by micromagnetic simulations. Finally, we show that the skyrmionic cocoons can be electrically detected using magneto-transport measurements.

Almost Perfect Spin Filtering in Graphene-Based Magnetic Tunnel Junctions.

We report on large spin-filtering effects in epitaxial graphene-based spin valves, strongly enhanced in our specific multilayer case. Our results were obtained by the effective association of chemical vapor deposited (CVD) multilayer graphene with a high quality epitaxial Ni(111) ferromagnetic spin source. We highlight that the Ni(111) spin source electrode crystallinity and metallic state are preserved and stabilized by multilayer graphene CVD growth. Complete nanometric spin valve junctions are fabricated using a local probe indentation process, and spin properties are extracted from the graphene-protected ferromagnetic electrode through the use of a reference Al2O3/Co spin analyzer. Strikingly, spin-transport measurements in these structures give rise to large negative tunnel magneto-resistance TMR = -160%, pointing to a particularly large spin polarization for the Ni(111)/Gr interface PNi/Gr, evaluated up to -98%. We then discuss an emerging physical picture of graphene-ferromagnet systems, sustained both by experimental data and ab initio calculations, intimately combining efficient spin filtering effects arising (i) from the bulk band structure of the graphene layers purifying the extracted spin direction, (ii) from the hybridization effects modulating the amplitude of spin polarized scattering states over the first few graphene layers at the interface, and (iii) from the epitaxial interfacial matching of the graphene layers with the spin-polarized Ni surface selecting well-defined spin polarized channels. Importantly, these main spin selection effects are shown to be either cooperating or competing, explaining why our transport results were not observed before. Overall, this study unveils a path to harness the full potential of low Resitance.Area (RA) graphene interfaces in efficient spin-based devices.

Combined spin filtering actions in hybrid magnetic junctions based on organic chains covalently attached to graphene.

We present a bias-controlled spin-filtering mechanism in spin-valves including a hybrid organic chain/graphene interface. Wet growth conditions of oligomeric molecular chains would usually lead, during standard CMOS-compatible fabrication processes, to the quenching of spintronics properties of metallic spin sources due to oxidation. We demonstrate by X-ray photoelectron spectroscopy that the use of a protective graphene layer fully preserves the metallic character of the ferromagnetic surface and thus its capability to deliver spin polarized currents. We focus here on a small aromatic chain of controllable lengths, formed by nitrobenzene monomers and derived from the commercial 4-nitrobenzene diazonium tetrafluoroborate, covalently attached to the graphene passivated spin sources thanks to electroreduction. A unique bias dependent switch of the spin signal is then observed in complete spin valve devices, from minority to majority spin carriers filtering. First-principles calculations are used to highlight the key role played by the spin-dependent hybridization of electronic states present at the different interfaces. Our work is a first step towards the exploration of spin transport using different functional molecular chains. It opens the perspective of atomic tailoring of magnetic junction devices towards spin and quantum transport control, thanks to the flexibility of ambient electrochemical surface functionalization processes.

Unveiling a Chemisorbed Crystallographically Heterogeneous Graphene/L10-FePd Interface with a Robust and Perpendicular Orbital Moment.

A crystallographically heterogeneous interface was fabricated by growing hexagonal graphene (Gr) using chemical vapor deposition (CVD) on a tetragonal FePd epitaxial film grown by magnetron sputtering. FePd was alternately arranged with Fe and Pd in the vertical direction, and the outermost surface atom was identified primarily as Fe rather than Pd. This means that FePd has a high degree of L10-ordering, and the outermost Fe bonds to the carbon of Gr at the interface. When Gr is grown by CVD, the crystal orientation of hexagonal Gr toward tetragonal L10-FePd selects an energetically stable structure based on the van der Waals (vdW) force. The atomic relationship of Gr/L10-FePd, which is an energetically stable interface, was unveiled theoretically and experimentally. The Gr armchair axis was parallel to FePd [100]L10, where Gr was under a small strain by chemical bonding. Focusing on the interatomic distance between the Gr and FePd layers, the distance was theoretically and experimentally determined to be approximately 0.2 nm. This shorter distance (≈0.2 nm) can be explained by the chemisorption-type vdW force of strong orbital hybridization, rather than the longer distance (≈0.38 nm) of the physisorption-type vdW force. Notably, depth-resolved X-ray magnetic circular dichroism analyses revealed that the orbital magnetic moment (Ml) of Fe in FePd emerged at the Gr/FePd interface (@inner FePd: Ml = 0.16 µB → @Gr/FePd interface: Ml = 0.32 µB). This interfacially enhanced Ml showed obvious anisotropy in the perpendicular direction, which contributed to interfacial perpendicular magnetic anisotropy (IPMA). Moreover, the interfacially enhanced Ml and interfacially enhanced electron density exhibited robustness. It is considered that the shortening of the interatomic distance produces a robust high electron density at the interface, resulting in a chemisorption-type vdW force and orbital hybridization. Eventually, the robust interfacial anisotropic Ml emerged at the crystallographically heterogeneous Gr/L10-FePd interface. From a practical viewpoint, IPMA is useful because it can be incorporated into the large bulk perpendicular magnetic anisotropy (PMA) of L10-FePd. A micromagnetic simulation assuming both PMA and IPMA predicted that perpendicularly magnetized magnetic tunnel junctions (p-MTJs) using Gr/L10-FePd could realize 10-year data retention in a small recording layer with a circular diameter and thickness of 10 and 2 nm, respectively. We unveiled the energetically stable atomic structure in the crystallographically heterogeneous interface, discovered the emergence of the robust IPMA, and predicted that the Gr/L10-FePd p-MTJ is significant for high-density X nm generation magnetic random-access memory (MRAM) applications.

X-ray magnetic dichroism and tunnel magneto-resistance study of the magnetic phase in epitaxial CrVOxnanoclusters.

Epitaxial clusters of chromium and chromium-vanadium oxides are studied by tunnel magneto-resistivity measurements, x-ray absorption spectrometry and circular magnetic circular dichroism. They turn out to carry a small magnetic moment that follows a super-paramagnetic behavior. The chromium ion contribution to this magnetization is mainly due to an original magnetic Cr2O3-like phase, whereas usual Cr2O3is known to be anti-ferromagnetic in the bulk. For mixed clusters, vanadium ions also contribute to the total magnetization and they are coupled to the chromium ion spins. By measuring the dichroic signal at different temperatures, we get insight into the possible spin configurations of vanadium and chromium ions: we propose that the magnetic dipoles observed in the clusters assembly could be related to ionic spins that couple at a very short range, as for instance in short one-dimensional spins chains.

Nonreciprocal Transport in a Rashba Ferromagnet, Delafossite PdCoO2.

Rashba interfaces yield efficient spin-charge interconversion and give rise to nonreciprocal transport phenomena. Here, we report magnetotransport experiments in few-nanometer-thick films of PdCoO2, a delafossite oxide known to display a large Rashba splitting and surface ferromagnetism. By analyzing the angle dependence of the first- and second-harmonic longitudinal and transverse resistivities, we identify a Rashba-driven unidirectional magnetoresistance that competes with the anomalous Nernst effect below the Curie point. We estimate a Rashba coefficient of 0.75 ± 0.3 eV Å and argue that our results qualify delafossites as a new family of oxides for nanospintronics and spin-orbitronics, beyond perovskite materials.

Band-Gap Landscape Engineering in Large-Scale 2D Semiconductor van der Waals Heterostructures.

We present a growth process relying on pulsed laser deposition for the elaboration of complex van der Waals heterostructures on large scales, at a 400 °C CMOS-compatible temperature. Illustratively, we define a multilayer quantum well geometry through successive in situ growths, leading to WSe2 being encapsulated into WS2 layers. The structural constitution of the quantum well geometry is confirmed by Raman spectroscopy combined with transmission electron microscopy. The large-scale high homogeneity of the resulting 2D van der Waals heterostructure is also validated by macro- and microscale Raman mappings. We illustrate the benefit of this integrative in situ approach by showing the structural preservation of even the most fragile 2D layers once encapsulated in a van der Waals heterostructure. Finally, we fabricate a vertical tunneling device based on these large-scale layers and discuss the clear signature of electronic transport controlled by the quantum well configuration with ab initio calculations in support. The flexibility of this direct growth approach, with multilayer stacks being built in a single run, allows for the definition of complex 2D heterostructures barely accessible with usual exfoliation or transfer techniques of 2D materials. Reminiscent of the III-V semiconductors' successful exploitation, our approach unlocks virtually infinite combinations of large 2D material families in any complex van der Waals heterostructure design.

Spin filtering by proximity effects at hybridized interfaces in spin-valves with 2D graphene barriers.

We report on spin transport in state-of-the-art epitaxial monolayer graphene based 2D-magnetic tunnel junctions (2D-MTJs). In our measurements, supported by ab-initio calculations, the strength of interaction between ferromagnetic electrodes and graphene monolayers is shown to fundamentally control the resulting spin signal. In particular, by switching the graphene/ferromagnet interaction, spin transport reveals magneto-resistance signal MR > 80% in junctions with low resistance × area products. Descriptions based only on a simple K-point filtering picture (i.e. MR increase with the number of layers) are not sufficient to predict the behavior of our devices. We emphasize that hybridization effects need to be taken into account to fully grasp the spin properties (such as spin dependent density of states) when 2D materials are used as ultimately thin interfaces. While this is only a first demonstration, we thus introduce the fruitful potential of spin manipulation by proximity effect at the hybridized 2D material / ferromagnet interface for 2D-MTJs.

Band-Structure Spin-Filtering in Vertical Spin Valves Based on Chemical Vapor Deposited WS2.

We report on spin transport in WS2-based 2D-magnetic tunnel junctions (2D-MTJs), unveiling a band structure spin filtering effect specific to the transition metal dichalcogenides (TMDCs) family. WS2 mono-, bi-, and trilayers are derived by a chemical vapor deposition process and further characterized by Raman spectroscopy, atomic force microscopy (AFM), and photoluminescence spectroscopy. The WS2 layers are then integrated in complete Co/Al2O3/WS2/Co MTJ hybrid spin-valve structures. We make use of a tunnel Co/Al2O3 spin analyzer to probe the extracted spin-polarized current from the WS2/Co interface and its evolution as a function of WS2 layer thicknesses. For monolayer WS2, our technological approach enables the extraction of the largest spin signal reported for a TMDC-based spin valve, corresponding to a spin polarization of PCo/WS2 = 12%. Interestingly, for bi- and trilayer WS2, the spin signal is reversed, which indicates a switch in the mechanism of interfacial spin extraction. With the support of ab initio calculations, we propose a model to address the experimentally measured inversion of the spin polarization based on the change in the WS2 band structure while going from monolayer (direct bandgap) to bilayer (indirect bandgap). These experiments illustrate the rich potential of the families of semiconducting 2D materials for the control of spin currents in 2D-MTJs.

Anisotropic Magneto-Coulomb Properties of 2D-0D Heterostructure Single Electron Device.

Fabrication and spintronics properties of 2D-0D heterostructures are reported. Devices based on graphene ("Gr")-aluminium nanoclusters heterostructures show robust and reproducible single-electron transport features, in addition to spin-dependent functionality when using a top magnetic electrode. The magnetic orientation of this single ferromagnetic electrode enables the modulation of the environmental charge experienced by the aluminium nanoclusters. This anisotropic magneto-Coulomb effect, originating from spin-orbit coupling within the ferromagnetic electrode, provides tunable spin valve-like magnetoresistance signatures without the requirement of spin coherent charge tunneling. These results extend the capability of Gr to act both as electrode and as a platform for the growth of 2D-0D mixed-dimensional van der Waals heterostructures, providing magnetic functionalities in the Coulomb blockade regime on scalable spintronic devices. These heterostructures pave the way towards novel device architectures at the crossroads of 2D material physics and spin electronics.

A Local Study of the Transport Mechanisms in MoS2 Layers for Magnetic Tunnel Junctions.

MoS2-based vertical spintronic devices have attracted an increasing interest thanks to theoretical predictions of large magnetoresistance signals. However, experimental performances are still far from expectations. Here, we carry out the local electrical characterization of thin MoS2 flakes in a Co/Al2O3/MoS2 structure through conductive tip AFM measurements. We show that thin MoS2 presents a metallic behavior with a strong lateral transport contribution that hinders the direct tunnelling through thin layers. Indeed, no resistance dependence is observed with the flake thickness. These findings reveal a spin depolarization source in the MoS2-based spin valves, thus pointing to possible solutions to improve their spintronic properties.

Insulator-to-Metallic Spin-Filtering in 2D-Magnetic Tunnel Junctions Based on Hexagonal Boron Nitride.

We report on the integration of atomically thin 2D insulating hexagonal boron nitride (h-BN) tunnel barriers into magnetic tunnel junctions (2D-MTJs) by fabricating two illustrative systems (Co/h-BN/Co and Co/h-BN/Fe) and by discussing h-BN potential for metallic spin filtering. The h-BN is directly grown by chemical vapor deposition on prepatterned Co and Fe stripes. Spin-transport measurements reveal tunnel magneto-resistances in these h-BN-based MTJs as high as 12% for Co/h-BN/h-BN/Co and 50% for Co/h-BN/Fe. We analyze the spin polarizations of h-BN/Co and h-BN/Fe interfaces extracted from experimental spin signals in light of spin filtering at hybrid chemisorbed/physisorbed h-BN, with support of ab initio calculations. These experiments illustrate the strong potential of h-BN for MTJs and are expected to ignite further investigations of 2D materials for large signal spin devices.

Conductance Oscillations in a Graphene/Nanocluster Hybrid Material: Toward Large-Area Single-Electron Devices.

Large assemblies of self-organized aluminum nanoclusters embedded in an oxide layer are formed on graphene templates and used to build tunnel-junction devices. Unexpectedly, single-electron-transport behavior with well-defined Coulomb oscillations is observed for a record junction area of up to 100 µm2 containing millions of metal islands. Such graphene-metal nanocluster hybrid materials offer new prospects for single-electron electronics.

Voltage-dependent magnetic phase transition in magneto-electric epitaxial Cr2O3 nanoclusters.

We observe, as a function of temperature, a second order magnetic phase transition in nanometric Cr2O3 clusters that are epitaxially embedded in an insulating MgO matrix. They are investigated through their tunnel magneto-resistance signature, the MgO layer being used as a tunnel barrier. We infer the small magnetic dipoles carried by the Cr2O3 clusters and provide evidence of a magnetic phase transition at low temperature in those clusters: they evolve from an anti ferromagnetic state, with zero net moment close to 0 K, to a weak ferromagnetic state that saturates above about 10 K. The influence of magneto-electric effects on the weak ferromagnetic phase is also striking: the second order transition temperature turns out to be linearly dependent on the applied electric field.

Epitaxy of MgO magnetic tunnel barriers on epitaxial graphene.

Epitaxial growth of electrodes and tunnel barriers on graphene is one of the main technological bottlenecks for graphene spintronics. In this paper, we demonstrate that MgO(111) epitaxial tunnel barriers, one of the prime candidates for spintronic application, can be grown by molecular beam epitaxy on epitaxial graphene on SiC(0001). Ferromagnetic metals (Fe, Co, Fe20Ni80) were epitaxially grown on top of the MgO barrier, thus leading to monocrystalline electrodes on graphene. Structural and magnetic characterizations were performed on these ferromagnetic metals after annealing and dewetting: they form clusters with a 100 nm typical lateral width, which are mostly magnetic monodomains in the case of Fe. This epitaxial stack opens the way to graphene spintronic devices taking benefits from a coherent tunnelling current through the epitaxial MgO/graphene stack.