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Ralph, Daniel C.

Publications and source records attributed to Ralph, Daniel C..

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 BiFeO 3 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 BiFeO 3 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 BiFeO 3 , an all-oxide, energy-scalable logic is demonstrated composed of spin-orbit injection, detection and magnetoelectric control. In conclusion, our observations open a new chapter of multiferroic magnons and pave another path towards low-dissipation nanoelectronics.

36 MATERIALS SCIENCE↗

Thermally generated spin current in the topological insulator Bi 2 Se 3

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 Bi 2 Se 3 /CoFeB. We find that Bi 2 Se 3 does generate substantial thermally driven spin currents. A lower bound for the ratio of spin current density to thermal gradient is $\frac{J_{s}}{∇_{x}T}$ = (4.9 ± 0.9) × 10 6 ($\frac{ℏ}{2e}$) $\frac{A m^{-2}}{K μm^{-1}}$, and a lower bound for the magnitude of the spin Nernst ratio is -0.61 ± 0.11. The spin Nernst ratio for Bi 2 Se 3 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 Bi 2 Se 3 can be understood via Mott relations to be due to an overall large spin Hall conductivity and its dependence on electron energy.

36 MATERIALS SCIENCE↗

Tuning the Curie temperature of a two-dimensional magnet/topological insulator heterostructure to above room temperature by epitaxial growth

Heterostructures of two-dimensional (2D) van der Waals (vdW) magnets and topological insulators (TI) are of substantial interest as candidate materials for efficient spin-torque switching, quantum anomalous Hall effect, and chiral spin textures. However, since many of the vdW magnets have Curie temperatures below room temperature, we want to understand how materials can be modified to stabilize their magnetic ordering to higher temperatures. In this work, we utilize molecular beam epitaxy to systematically tune the Curie temperature (T C ) in thin film Fe 3 GeTe 2 /Bi 2 Te 3 from bulklike values (~220 K) to above room temperature by increasing the growth temperature from 300°C to 375°C. For samples grown at 375°C, cross-sectional scanning transmission electron microscopy (STEM) reveals the spontaneous formation of different Fe m Ge n Te 2 compositions (e.g., Fe 5 Ge 2 Te 2 and Fe 7 Ge 6 Te 2 ) as well as intercalation in the vdW gaps, which are possible origins of the enhanced Curie temperature. Furthermore, this observation paves the way for developing various Fe m Ge n Te 2 /TI heterostructures with novel properties.

36 MATERIALS SCIENCE↗

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. Additionally, 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.

36 MATERIALS SCIENCE↗

Symmetry Control of Unconventional Spin–Orbit Torques in IrO 2

Abstract 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 (IrO 2 ), 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 IrO 2 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.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

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. Here, 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.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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 devices. Facilitating a deeper understanding of sub-100 nm to atomic-scale spin textures requires more advanced magnetic imaging techniques. Here, we demonstrate a Lorentz electron ptychography (LEP) method which can enable high-resolution, high-sensitivity magnetic field imaging for widely-available electron microscopes. The resolution of LEP is not limited by the usual diffraction limit of the 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 to 6 times depending on the allowable dose. Using FeGe as a 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 effects from the imaging optics via LEP. 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 the nanoscale spin textures, especially magnetization discontinuities and topological defects in nanomagnets. In conclusion, 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 magnets.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Tilted spin current generated by the collinear antiferromagnet ruthenium dioxide

Symmetry plays a central role in determining the polarization of spin currents induced by electric fields. It also influences how these spin currents generate spin-transfer torques in magnetic devices. Here, we show that an out-of-plane damping-like torque can be generated in ruthenium oxide (RuO 2 )/permalloy devices when the Néel vector of the collinear antiferromagnet RuO 2 is canted relative to the sample plane. By measuring characteristic changes in all three components of the electric-field-induced torque vector as a function of the angle of the electric field relative to the crystal axes, we find that the RuO 2 generates a spin current with a well-defined tilted spin orientation that is approximately parallel to the Néel vector. A maximum out-of-plane damping-like spin torque efficiency per unit electric field of 7±1 × 10 3 Ω -1 m -1 is measured at room temperature. Here, the observed angular dependence indicates that this is an antiferromagnetic spin Hall effect with symmetries that are distinct from other mechanisms of spin-current generation reported in antiferromagnetic and ferromagnetic materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Origin of transverse voltages generated by thermal gradients and electric fields in ferrimagnetic-insulator/heavy-metal bilayers

We compare thermal-gradient-driven transverse voltages in ferrimagnetic-insulator/heavy-metal bilayers (Tm 3 Fe 5 O 12 /W and Tm 3 Fe 5 O 12 /Pt) to corresponding electrically driven transverse resistances at and above room temperature. We find for Tm 3 Fe 5 O 12 /W that the thermal and electrical effects can be explained by a common spin-current detection mechanism, the physics underlying spin Hall magnetoresistance (SMR). However, for Tm 3 Fe 5 O 12 /Pt the ratio of the electrically driven transverse voltages (planar Hall signal/anomalous Hall signal) is much larger than the ratio of corresponding thermal-gradient signals, a result which is very different from expectations for a SMR-based mechanism alone. Here, we ascribe this difference to a proximity-induced magnetic layer at the Tm 3 Fe 5 O 12 /Pt interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Separation of Artifacts from Spin–Torque Ferromagnetic Resonance Measurements of Spin–Orbit Torque for the Low–Symmetry Van der Waals Semi–Metal ZrTe 3

Spin-orbit torques generated by exfoliated layers of the low-symmetry semi-metal ZrTe 3 are measured using the spin-torque ferromagnetic resonance (ST-FMR) technique. When the ZrTe 3 has a thickness greater than about 10 nm, artifacts due to spin pumping and/or resonant heating can cause the standard ST-FMR analysis to overestimate the true magnitude of the torque efficiency by as much as a factor of 30, and to indicate incorrectly that the spin-orbit torque depends strongly on the ZrTe 3 layer thickness. Artifact-free measurements can still be achieved over a substantial thickness range by the method developed recently to detect ST-FMR signals in the Hall geometry as well as the longitudinal geometry. ZrTe 3 /Permalloy samples generate a conventional in-plane anti-damping spin torque efficiency ξ$^{FL}_{∥}$ = 0.014 ± 0.004, and an unconventional in-plane field-like torque efficiency |ξ$^{FL}_{∥}$| = 0.003 ± 0.001. As a result, the out-of-plane anti-damping torque is negligible. It is suggested that artifacts similarly interfere with the standard ST-FMR analysis for other van der Waals samples thicker than about 10 nm.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Resolving Discrepancies in Spin-Torque Ferromagnetic Resonance Measurements: Lineshape versus Linewidth Analyses

When spin-orbit torques are measured using spin-torque ferromagnetic resonance, two alternative ways of analyzing the results to extract the torque efficiencies—lineshape analysis and analysis of the change in linewidth versus direct current—often give inconsistent results. We identify a source for these inconsistencies. We show that fits of spin-torque ferromagnetic resonance data to the standard analysis framework leave significant residuals that we identify as due to (i) current-induced excitations of a small volume of magnetic material with magnetic damping much larger than that of the bulk of the magnetic layer, which we speculate is associated with the heavy-metal–magnet interface and (ii) oscillations of the sample magnetization at the modulation frequency due to heating. Here, the dependence of the residual signals on direct current can interfere with an accurate extraction of spin-torque efficiencies by the linewidth method. We show that the discrepancies between the two types of analysis can be largely eliminated by extrapolation of the window of magnetic fields used in the linewidth fits to small values so as to minimize the influence of the residual signals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗