Manipulating chiral spin transport with ferroelectric polarization.

A magnon is a collective excitation of the spin structure in a magnetic insulator and can transmit spin angular momentum with negligible dissipation. This quantum of a spin wave has always been manipulated through magnetic dipoles (that is, by breaking time-reversal symmetry). Here we report the experimental observation of chiral spin transport in multiferroic BiFeO3 and its control by reversing the ferroelectric polarization (that is, by breaking spatial inversion symmetry). The ferroelectrically controlled magnons show up to 18% modulation at room temperature. The spin torque that the magnons in BiFeO3 carry can be used to efficiently switch the magnetization of adjacent magnets, with a spin-torque efficiency comparable to the spin Hall effect in heavy metals. Utilizing such controllable magnon generation and transmission in BiFeO3, an all-oxide, energy-scalable logic is demonstrated composed of spin-orbit injection, detection and magnetoelectric control. Our observations open a new chapter of multiferroic magnons and pave another path towards low-dissipation nanoelectronics.

Exchange Bias Between van der Waals Materials: Tilted Magnetic States and Field-Free Spin-Orbit-Torque Switching.

Magnetic van der Waals heterostructures provide a unique platform to study magnetism and spintronics device concepts in the 2D limit. Here, studies of exchange bias from the van der Waals antiferromagnet CrSBr acting on the van der Waals ferromagnet Fe3GeTe2 (FGT) are reported. The orientation of the exchange bias is along the in-plane easy axis of CrSBr, perpendicular to the out-of-plane anisotropy of the FGT, inducing a strongly tilted magnetic configuration in the FGT. Furthermore, the in-plane exchange bias provides sufficient symmetry breaking to allow deterministic spin-orbit torque switching of the FGT in CrSBr/FGT/Pt samples at zero applied magnetic field. A minimum thickness of the CrSBr of >10 nm is needed to provide a non-zero exchange bias at 30 K.

Thermally generated spin current in the topological insulator Bi2Se3.

We present measurements of thermally generated transverse spin currents in the topological insulator Bi2Se3, thereby completing measurements of interconversions among the full triad of thermal gradients, charge currents, and spin currents. We accomplish this by comparing the spin Nernst magneto-thermopower to the spin Hall magnetoresistance for bilayers of Bi2Se3/CoFeB. We find that Bi2Se3 does generate substantial thermally driven spin currents. A lower bound for the ratio of spin current density to thermal gradient is [Formula: see text] = (4.9 ± 0.9) × 106 [Formula: see text], and a lower bound for the magnitude of the spin Nernst ratio is -0.61 ± 0.11. The spin Nernst ratio for Bi2Se3 is the largest among all materials measured to date, two to three times larger compared to previous measurements for the heavy metals Pt and W. Strong thermally generated spin currents in Bi2Se3 can be understood via Mott relations to be due to an overall large spin Hall conductivity and its dependence on electron energy.

Sagnac interferometry for high-sensitivity optical measurements of spin-orbit torque.

Sagnac interferometry can provide a substantial improvement in signal-to-noise ratio compared to conventional magnetic imaging based on the magneto-optical Kerr effect. We show that this improvement is sufficient to allow quantitative measurements of current-induced magnetic deflections due to spin-orbit torque even in thin-film magnetic samples with perpendicular magnetic anisotropy, for which the Kerr rotation is second order in the magnetic deflection. Sagnac interferometry can also be applied beneficially for samples with in-plane anisotropy, for which the Kerr rotation is first order in the deflection angle. Optical measurements based on Sagnac interferometry can therefore provide a cross-check on electrical techniques for measuring spin-orbit torque. Different electrical techniques commonly give quantitatively inconsistent results so that Sagnac interferometry can help to identify which techniques are affected by unidentified artifacts.

Symmetry Control of Unconventional Spin-Orbit Torques in IrO2.

Spin-orbit torques generated by a spin current are key to magnetic switching in spintronic applications. The polarization of the spin current dictates the direction of switching required for energy-efficient devices. Conventionally, the polarizations of these spin currents are restricted to be along a certain direction due to the symmetry of the material allowing only for efficient in-plane magnetic switching. Unconventional spin-orbit torques arising from novel spin current polarizations, however, have the potential to switch other magnetization orientations such as perpendicular magnetic anisotropy, which is desired for higher density spintronic-based memory devices. Here, it is demonstrated that low crystalline symmetry is not required for unconventional spin-orbit torques and can be generated in a nonmagnetic high symmetry material, iridium dioxide (IrO2 ), using epitaxial design. It is shown that by reducing the relative crystalline symmetry with respect to the growth direction large unconventional spin currents can be generated and hence spin-orbit torques. Furthermore, the spin polarizations detected in (001), (110), and (111) oriented IrO2 thin films are compared to show which crystal symmetries restrict unconventional spin transport. Understanding and tuning unconventional spin transport generation in high symmetry materials can provide a new route towards energy-efficient magnetic switching in spintronic devices.

Synthesis, Hole Doping, and Electrical Properties of a Semiconducting Azatriangulene-Based Covalent Organic Framework.

Two-dimensional covalent organic frameworks (2D COFs) containing heterotriangulenes have been theoretically identified as semiconductors with tunable, Dirac-cone-like band structures, which are expected to afford high charge-carrier mobilities ideal for next-generation flexible electronics. However, few bulk syntheses of these materials have been reported, and existing synthetic methods provide limited control of network purity and morphology. Here, we report transimination reactions between benzophenone-imine-protected azatriangulenes (OTPA) and benzodithiophene dialdehydes (BDT), which afforded a new semiconducting COF network, OTPA-BDT. The COFs were prepared as both polycrystalline powders and thin films with controlled crystallite orientation. The azatriangulene nodes are readily oxidized to stable radical cations upon exposure to an appropriate p-type dopant, tris(4-bromophenyl)ammoniumyl hexachloroantimonate, after which the network's crystallinity and orientation are maintained. Oriented, hole-doped OTPA-BDT COF films exhibit electrical conductivities of up to 1.2 × 10-1 S cm-1, which are among the highest reported for imine-linked 2D COFs to date.

A puzzling insensitivity of magnon spin diffusion to the presence of 180-degree domain walls.

We present room-temperature measurements of magnon spin diffusion in epitaxial ferrimagnetic insulator MgAl0.5Fe1.5O4 (MAFO) thin films near zero applied magnetic field where the sample forms a multi-domain state. Due to a weak uniaxial magnetic anisotropy, the domains are separated primarily by 180° domain walls. We find, surprisingly, that the presence of the domain walls has very little effect on the spin diffusion - nonlocal spin transport signals in the multi-domain state retain at least 95% of the maximum signal strength measured for the spatially-uniform magnetic state, over distances at least five times the typical domain size. This result is in conflict with simple models of interactions between magnons and static domain walls, which predict that the spin polarization carried by the magnons reverses upon passage through a 180° domain wall.

Strong variation of spin-orbit torques with relative spin relaxation rates in ferrimagnets.

Spin-orbit torques (SOTs) have been widely understood as an interfacial transfer of spin that is independent of the bulk properties of the magnetic layer. Here, we report that SOTs acting on ferrimagnetic FexTb1-x layers decrease and vanish upon approaching the magnetic compensation point because the rate of spin transfer to the magnetization becomes much slower than the rate of spin relaxation into the crystal lattice due to spin-orbit scattering. These results indicate that the relative rates of competing spin relaxation processes within magnetic layers play a critical role in determining the strength of SOTs, which provides a unified understanding for the diverse and even seemingly puzzling SOT phenomena in ferromagnetic and compensated systems. Our work indicates that spin-orbit scattering within the magnet should be minimized for efficient SOT devices. We also find that the interfacial spin-mixing conductance of interfaces of ferrimagnetic alloys (such as FexTb1-x) is as large as that of 3d ferromagnets and insensitive to the degree of magnetic compensation.

Lorentz electron ptychography for imaging magnetic textures beyond the diffraction limit.

Nanoscale spin textures, especially magnetic skyrmions, have attracted intense interest as candidate high-density and power-efficient information carriers for spintronic devices1,2. Facilitating a deeper understanding of sub-hundred-nanometre to atomic-scale spin textures requires more advanced magnetic imaging techniques3-5. Here we demonstrate a Lorentz electron ptychography method that can enable high-resolution, high-sensitivity magnetic field imaging for widely available electron microscopes. The resolution of Lorentz electron ptychography is not limited by the usual diffraction limit of lens optics, but instead is determined by the maximum scattering angle at which a statistically meaningful dose can still be recorded-this can be an improvement of up to 2-6 times depending on the allowable dose. Using FeGe as the model system, we realize a more accurate magnetic field measurement of skyrmions with an improved spatial resolution and sensitivity by also correcting the probe-damping effect from the imaging optics via Lorentz electron ptychography. This allows us to directly resolve subtle internal structures of magnetic skyrmions near the skyrmion cores, boundaries and dislocations in an FeGe single crystal. Our study establishes a quantitative, high-resolution magnetic microscopy technique that can reveal nanoscale spin textures, especially magnetization discontinuities and topological defects in nanomagnets6. The technique's high-dose efficiency should also make it well suited for the exploration of magnetic textures in electron radiation-sensitive materials such as organic or molecular magnets7.

Anisotropic Gigahertz Antiferromagnetic Resonances of the Easy-Axis van der Waals Antiferromagnet CrSBr.

We report measurements of antiferromagnetic resonances in the van der Waals easy-axis antiferromagnet CrSBr. The interlayer exchange field and magnetocrystalline anisotropy fields are comparable to laboratory magnetic fields, allowing a rich variety of gigahertz-frequency dynamical modes to be accessed. By mapping the resonance frequencies as a function of the magnitude and angle of applied magnetic field, we identify the different regimes of antiferromagnetic dynamics. The spectra show good agreement with a Landau-Lifshitz model for two antiferromagnetically coupled sublattices, accounting for interlayer exchange and triaxial magnetic anisotropy. Fits allow us to quantify the parameters governing the magnetic dynamics: At 5 K, the interlayer exchange field is µ0HE = 0.395(2) T, and the hard and intermediate-axis anisotropy parameters are µ0Hc = 1.30(2) T and µ0Ha = 0.383(7) T. The existence of within-plane anisotropy makes it possible to control the degree of hybridization between the antiferromagnetic resonances using an in-plane magnetic field.

Gate-Tunable Anomalous Hall Effect in a 3D Topological Insulator/2D Magnet van der Waals Heterostructure.

We demonstrate advantages of samples made by mechanical stacking of exfoliated van der Waals materials for controlling the topological surface state of a three-dimensional topological insulator (TI) via interaction with an adjacent magnet layer. We assemble bilayers with pristine interfaces using exfoliated flakes of the TI BiSbTeSe2 and the magnet Cr2Ge2Te6, thereby avoiding problems caused by interdiffusion that can affect interfaces made by top-down deposition methods. The samples exhibit an anomalous Hall effect (AHE) with abrupt hysteretic switching. For the first time in samples composed of a TI and a separate ferromagnetic layer, we demonstrate that the amplitude of the AHE can be tuned via gate voltage with a strong peak near the Dirac point. This is the signature expected for the AHE due to Berry curvature associated with an exchange gap induced by interaction between the topological surface state and an out-of-plane-oriented magnet.

Anisotropic Magnon Spin Transport in Ultrathin Spinel Ferrite Thin Films─Evidence for Anisotropy in Exchange Stiffness.

Magnon-mediated spin flow in magnetically ordered insulators enables long-distance spin-based information transport with low dissipation. In the materials studied to date, no anisotropy has been observed in the magnon propagation length as a function of propagation direction. Here, we report measurements of magnon spin transport in a spinel ferrite, magnesium aluminum ferrite MgAl0.5Fe1.5O4 (MAFO), which has a substantial in-plane 4-fold magnetic anisotropy. We observe spin diffusion lengths > 0.8 µm at room temperature in 6 nm films, with spin diffusion lengths 30% longer along the easy axes compared to the hard axes. The sign of this difference is opposite to the effects just of anisotropy in the magnetic energy for a uniform magnetic state. We suggest instead that accounting for anisotropy in exchange stiffness is necessary to explain these results. These findings provide an approach for controlling magnon transport via strain, which opens new opportunities for designing magnonic devices.

Novel Spin-Orbit Torque Generation at Room Temperature in an All-Oxide Epitaxial La0.7 Sr0.3 MnO3 /SrIrO3 System.

Spin-orbit torques (SOTs) that arise from materials with large spin-orbit coupling offer a new pathway for energy-efficient and fast magnetic information storage. SOTs in conventional heavy metals and topological insulators are explored extensively, while 5d transition metal oxides, which also host ions with strong spin-orbit coupling, are a relatively new territory in the field of spintronics. An all-oxide, SrTiO3 (STO)//La0.7 Sr0.3 MnO3 (LSMO)/SrIrO3 (SIO) heterostructure with lattice-matched crystal structure is synthesized, exhibiting an epitaxial and atomically sharp interface between the ferromagnetic LSMO and the high spin-orbit-coupled metal SIO. Spin-torque ferromagnetic resonance (ST-FMR) is used to probe the effective magnetization and the SOT efficiency in LSMO/SIO heterostructures grown on STO substrates. Remarkably, epitaxial LSMO/SIO exhibits a large SOT efficiency, ξ||  = 1, while retaining a reasonably low shunting factor and increasing the effective magnetization of LSMO by ≈50%. The findings highlight the significance of epitaxy as a powerful tool to achieve a high SOT efficiency, explore the rich physics at the epitaxial interface, and open up a new pathway for designing next-generation energy-efficient spintronic devices.

Electronically Coupled 2D Polymer/MoS2 Heterostructures.

Emergent quantum phenomena in electronically coupled two-dimensional heterostructures are central to next-generation optical, electronic, and quantum information applications. Tailoring electronic band gaps in coupled heterostructures would permit control of such phenomena and is the subject of significant research interest. Two-dimensional polymers (2DPs) offer a compelling route to tailored band structures through the selection of molecular constituents. However, despite the promise of synthetic flexibility and electronic design, fabrication of 2DPs that form electronically coupled 2D heterostructures remains an outstanding challenge. Here, we report the rational design and optimized synthesis of electronically coupled semiconducting 2DP/2D transition metal dichalcogenide van der Waals heterostructures, demonstrate direct exfoliation of the highly crystalline and oriented 2DP films down to a few nanometers, and present the first thickness-dependent study of 2DP/MoS2 heterostructures. Control over the 2DP layers reveals enhancement of the 2DP photoluminescence by two orders of magnitude in ultrathin sheets and an unexpected thickness-dependent modulation of the ultrafast excited state dynamics in the 2DP/MoS2 heterostructure. These results provide fundamental insight into the electronic structure of 2DPs and present a route to tune emergent quantum phenomena in 2DP hybrid van der Waals heterostructures.

Effects of Anisotropic Strain on Spin-Orbit Torque Produced by the Dirac Nodal Line Semimetal IrO2.

We report spin-torque ferromagnetic resonance studies of the efficiency of the damping-like (ξDL) spin-orbit torque exerted on an adjacent ferromagnet film by current flowing in epitaxial (001) and (110) IrO2 thin films. IrO2 possesses Dirac nodal lines (DNLs) in the band structure that are gapped by spin-orbit coupling, which could enable a very high spin Hall conductivity, σSH. We find that the (001) films do exhibit exceptionally high ξDL ranging from 0.45 at 293 K to 0.65 at 30 K, which sets the lower bounds of σSH to be 1.9 × 105 and 3.75 × 105 Ω-1 m-1, respectively, 10 times higher and of opposite sign than the theoretical prediction. Furthermore, ξDL and σSH are substantially reduced in anisotropically strained (110) films. We suggest that this high sensitivity to anisotropic strain is because of changes in contributions to σSH near the DNLs.

Direct Visualization of Trimerized States in 1T

Transition-metal dichalcogenides containing tellurium anions show remarkable charge-lattice modulated structures and prominent interlayer character. Using cryogenic scanning transmission electron microscopy (STEM), we map the atomic-scale structures of the high temperature (HT) and low temperature (LT) modulated phases in 1T^{'}-TaTe_{2}. At HT, we directly show in-plane metal distortions which form trimerized clusters and staggered, three-layer stacking. In the LT phase at 93 K, we visualize an additional trimerization of Ta sites and subtle distortions of Te sites by extracting structural information from contrast modulations in plan-view STEM data. Coupled with density functional theory calculations and image simulations, this approach opens the door for atomic-scale visualizations of low temperature phase transitions and complex displacements in a variety of layered systems.

Manipulation of the van der Waals Magnet Cr2Ge2Te6 by Spin-Orbit Torques.

We report measurements of current-induced thermoelectric and spin-orbit torque effects within devices in which multilayers of the semiconducting two-dimensional van der Waals magnet Cr2Ge2Te6 (CGT) are integrated with Pt and Ta metal overlayers. We show that the magnetic orientation of the CGT can be detected accurately either electrically (using an anomalous Hall effect) or optically (using magnetic circular dichroism) with good consistency. The samples exhibit large thermoelectric effects, but nevertheless, the spin-orbit torque can be measured quantitatively using the angle-dependent second harmonic Hall technique. For CGT/Pt, we measure the spin-orbit torque efficiency to be similar to conventional metallic-ferromagnet/Pt devices with the same Pt resistivity. The interfacial transparency for spin currents is therefore similar in both classes of devices. Our results demonstrate the promise of incorporating semiconducting 2D magnets within spin-orbitronic and magneto-thermal devices.

Local Photothermal Control of Phase Transitions for On-Demand Room-Temperature Rewritable Magnetic Patterning.

The ability to make controlled patterns of magnetic structures within a nonmagnetic background is essential for several types of existing and proposed technologies. Such patterns provide the foundation of magnetic memory and logic devices, allow the creation of artificial spin-ice lattices, and enable the study of magnon propagation. Here, a novel approach for magnetic patterning that allows repeated creation and erasure of arbitrary shapes of thin-film ferromagnetic structures is reported. This strategy is enabled by epitaxial Fe0.52 Rh0.48 thin films designed so that both ferromagnetic and antiferromagnetic phases are bistable at room temperature. Starting with the film in a uniform antiferromagnetic state, the ability to write arbitrary patterns of the ferromagnetic phase is demonstrated by local heating with a focused laser. If desired, the results can then be erased by cooling below room temperature and the material repeatedly re-patterned.

Effective Spin-Mixing Conductance of Heavy-Metal-Ferromagnet Interfaces.

The effective spin-mixing conductance (G_{eff}^{↑↓}) of a heavy-metal-ferromagnet (HM-FM) interface characterizes the efficiency of the interfacial spin transport. Accurately determining G_{eff}^{↑↓} is critical to the quantitative understanding of measurements of direct and inverse spin Hall effects. G_{eff}^{↑↓} is typically ascertained from the inverse dependence of magnetic damping on the FM thickness under the assumption that spin pumping is the dominant mechanism affecting this dependence. We report that this assumption fails badly in many in-plane magnetized prototypical HM-FM systems in the nanometer-scale thickness regime. Instead, the majority of the damping is from two-magnon scattering at the FM interface, while spin-memory-loss scattering at the interface can also be significant. If these two effects are neglected, the results will be an unphysical "giant" apparent G_{eff}^{↑↓} and hence considerable underestimation of both the spin Hall ratio and the spin Hall conductivity in inverse or direct spin Hall experiments.

Variation of the giant intrinsic spin Hall conductivity of Pt with carrier lifetime.

More than a decade after the first theoretical and experimental studies of the spin Hall conductivity (SHC) of Pt, both its dominant origin and amplitude remain in dispute. We report the experimental determination of the rapid variation of the intrinsic SHC of Pt with the carrier lifetime (τ) in the dirty-metal regime by incorporating finely dispersed MgO intersite impurities into the Pt, while maintaining its essential band structure. This conclusively validates the theoretical prediction that the SHC in Pt in the dirty-metal regime should be dominated by the intrinsic contribution, and should decrease rapidly with shortening τ. When interfacial spin backflow is taken into account, the intrinsic SHC of Pt in the clean limit is at least 1.6 × 106 (ℏ/2e) ohm-1 m-1, more than 3.5 times greater than the available theoretical predictions. Our work also establishes a compelling spin Hall metal Pt0.6(MgO)0.4 with an internal giant spin Hall ratio of 0.73.