Metal-Free Organic Radical Spin Source.

Organic radicals have long been suggested as candidates for organic magnets and components in organic spintronic devices. Herein, we demonstrate spin current emission from an organic radical film via spin pumping at room temperature. We present the synthesis and the thin film preparation of a Blatter-type radical with outstanding stability and low roughness. These features enable the fabrication of a radical/ferromagnet bilayer, in which the spin current emission from the organic radical layer can be reversibly reduced when the ferromagnetic film is brought into simultaneous resonance with the radical. The results provide an experimental demonstration of a metal-free organic radical layer operating as a spin source, opening a new avenue for the development of purely organic spintronic devices and bridging the gap between potential and real applications.

Magnon Confinement in an All-on-Chip YIG Cavity Resonator Using Hybrid YIG/Py Magnon Barriers.

Confining magnons in cavities can introduce new functionalities to magnonic devices, enabling future magnonic structures to emulate the established photonic and electronic components. As a proof-of-concept, we report magnon confinement in a lithographically defined all-on-chip YIG cavity created between two YIG/Permalloy bilayers. We take advantage of the modified magnetic properties of the covered/uncovered YIG film to define on-chip distinct regions with boundaries capable of confining magnons. We confirm this by measuring multiple spin-pumping voltage peaks in a 400 nm wide platinum strip placed along the center of the cavity. These peaks coincide with multiple spin-wave resonance modes calculated for a YIG slab with the corresponding geometry. The fabrication of micrometer-sized YIG cavities following this technique represents a new approach to control coherent magnons, while the spin-pumping voltage in a nanometer-sized Pt strip demonstrates to be a noninvasive local detector of the magnon resonance intensity.

Sizable spin-to-charge conversion in PLD-grown amorphous (Mo, W)Te2-xfilms.

We report on the spin-to-charge conversion (SCC) in Mo0.25W0.75Te2-x(MWT)/Y3Fe5O12(YIG) heterostructures at room temperature. The centimeter-scale amorphous MWT films are deposited on liquid-phase-epitaxial YIG by pulsed laser deposition technique. The significant SCC voltage is measured in the MWT layer with a sizable spin Hall angle of ∼0.021 by spin pumping experiments. The control experiments by inserting MgO or Ag layer between MWT and YIG show that the SCC is mainly attributed to the inverse spin Hall effect rather than the thermal or interfacial Rashba effect. Our work provides a novel spin-source material for energy-efficient topological spintronic devices.

Spin pumping through nanocrystalline topological insulators.

The topological surface states (TSSs) in topological insulators (TIs) offer exciting prospects for dissipationless spin transport. Common spin-based devices, such as spin valves, rely on trilayer structures in which a non-magnetic layer is sandwiched between two ferromagnetic (FM) layers. The major disadvantage of using high-quality single-crystalline TI films in this context is that a single pair of spin-momentum locked channels spans across the entire film, meaning that only a very small spin current can be pumped from one FM to the other, along the side walls of the film. On the other hand, using nanocrystalline TI films, in which the grains are large enough to avoid hybridization of the TSSs, will effectively increase the number of spin channels available for spin pumping. Here, we used an element-selective, x-ray based ferromagnetic resonance technique to demonstrate spin pumping from a FM layer at resonance through the TI layer and into the FM spin sink.

The Giant Spin-to-Charge Conversion of the Layered Rashba Material BiTeI.

Rashba spin-orbit coupling (SOC) could facilitate an efficient interconversion between spin and charge currents. Among various systems, BiTeI holds one of the largest Rashba-type spin splittings. Unlike other Rashba systems (e.g., Bi/Ag and Bi2Se3), an experimental investigation of the spin-to-charge interconversion in BiTeI remains to be explored. Through performing an angle-resolved photoemission spectroscopy (ARPES) measurement, such a large Rashba-type spin splitting with a Rashba parameter αR = 3.68 eV Å is directly identified. By studying the spin pumping effect in the BiTeI/NiFe bilayer, we reveal a very large inverse Rashba-Edelstein length λIREE ≈ 1.92 nm of BiTeI at room temperature. Furthermore, the λIREE monotonously increases to 5.00 nm at 60 K, indicating an enhanced Rashba SOC at low temperature. These results suggest that BiTeI films with the giant Rashba SOC are promising for achieving efficient spin-to-charge interconversion, which could be implemented for building low-power-consumption spin-orbitronic devices.

Atomic Scale Control of Spin Current Transmission at Interfaces.

Ferromagnet/heavy metal bilayers represent a central building block for spintronic devices where the magnetization of the ferromagnet can be controlled by spin currents generated in the heavy metal. The efficiency of spin current generation is paramount. Equally important is the efficient transfer of this spin current across the ferromagnet/heavy metal interface. Here, we show theoretically and experimentally that for Ta as heavy metal the interface only partially transmits the spin current while this effect is absent when Pt is used as heavy metal. This is due to magnetic moment reduction at the interface caused by 3d-5d hybridization effects. We show that this effect can be avoided by atomically thin interlayers. On the basis of our theoretical model we conclude that this is a general effect and occurs for all 5d metals with less than half-filled 5d shell.

Chemical Approach Towards Broadband Spintronics on Nanoscale Pyrene Films.

The injection of pure spin current into the non-magnetic layer plays a crucial role in transmitting, processing, and storing data information in the realm of spintronics. To understand broadband molecular spintronics, pyrene oligomer film (≈20 nm thickness) was prepared using an electrochemical method forming indium tin oxide (ITO) electrode/pyrene covalent interfaces. Permalloy (Ni80 Fe20 ) films with different nanoscale thicknesses were used as top contact over ITO/pyrene layers to estimate the spin pumping efficiency across the interfaces using broadband ferromagnetic resonance spectra. The spintronic devices are composed of permalloy/pyrene/ITO orthogonal configuration, showing remarkable spin pumping from permalloy to pyrene film. The large spin pumping is evident from the linewidth broadening of 5.4 mT at 9 GHz, which is direct proof of spin angular momentum transfer across the interface. A striking observation is made with the high spin-mixing conductance of ≈1.02×1018  m-2 , a value comparable to the conventional heavy metals. Large spin angular moment transfer was observed at the permalloy-pyrene interfaces, especially at the lower thickness of permalloy, indicating a strong spinterface effect. Pure spin current injection from ferromagnetic into electrochemically grown pyrene films ensures efficient broadband spin transport, which opens a new area in molecular broadband spintronics.

Heavy metal deposition temperature tuned spin pumping efficiency control in permalloy/tantalum bilayers.

Spin pumping is a key property for spintronic application that can be realized in heavy metal/ferromagnet bilayers. Here we demonstrate the possibility of improving spin pumping in permalloy (Py)/tantalum (Ta) bilayers through control of Ta heavy metal deposition temperature. Through a combination of structural and ferromagnetic resonance based magnetization dynamics study, we reveal the role of Ta deposition temperature in improving spin mixing conductance which is a key parameter for spin pumping across the Py/Ta interface. The results show that by depositing Ta above room temperature, a high spin mixing conductance of 7.7 ×1018m-2is obtained withα-Ta layer. The results present an understanding of the correlation between heavy metal deposition temperature and interface structure improvement and consequent control of spin pumping in Py/Ta bilayers.

Dynamics of frequency-swept nuclear spin optical pumping in powdered diamond at low magnetic fields.

A broad effort is underway to improve the sensitivity of NMR through the use of dynamic nuclear polarization. Nitrogen vacancy (NV) centers in diamond offer an appealing platform because these paramagnetic defects can be optically polarized efficiently at room temperature. However, work thus far has been mainly limited to single crystals, because most polarization transfer protocols are sensitive to misalignment between the NV and magnetic field axes. Here we study the spin dynamics of NV-13C pairs in the simultaneous presence of optical excitation and microwave frequency sweeps at low magnetic fields. We show that a subtle interplay between illumination intensity, frequency sweep rate, and hyperfine coupling strength leads to efficient, sweep-direction-dependent 13C spin polarization over a broad range of orientations of the magnetic field. In particular, our results strongly suggest that finely tuned, moderately coupled nuclear spins are key to the hyperpolarization process, which makes this mechanism distinct from other known dynamic polarization channels. These findings pave the route to applications where powders are intrinsically advantageous, including the hyperpolarization of target fluids in contact with the diamond surface or the use of hyperpolarized particles as contrast agents for in vivo imaging.

Nonlocal Uniform-Mode Ferromagnetic Resonance Spin Pumping.

Nonlocal spin transport using lateral structures is attractive for spintronic devices. Typically, a spin current is generated by a ferromagnetic (FM) or a heavy metal (HM) electrode in a nonlocal structure, which can be detected by another FM or HM electrode. Here, we report a new nonlocal spin injection scheme using uniform-mode ferromagnetic resonance (FMR) spin pumping in Pt/Y3Fe5O12 (YIG) lateral structures. This scheme is enabled by well-separated resonant fields of Pt/YIG and bare YIG due to substantial change of anisotropy in YIG films induced by a Pt overlayer, allowing for clearly distinguishable local and nonlocal spin pumping. Our results show that the spin decay length of nonlocal uniform-mode spin pumping in 20 nm YIG films is 2.1 µm at room temperature.

Element-Specific Detection of Sub-Nanosecond Spin-Transfer Torque in a Nanomagnet Ensemble.

Spin currents can exert spin-transfer torques on magnetic systems even in the limit of vanishingly small net magnetization, as recently shown for antiferromagnets. Here, we experimentally show that a spin-transfer torque is operative in a macroscopic ensemble of weakly interacting, randomly magnetized Co nanomagnets. We employ element- and time-resolved X-ray ferromagnetic resonance (XFMR) spectroscopy to directly detect subnanosecond dynamics of the Co nanomagnets, excited into precession with cone angle ≳0.003° by an oscillating spin current. XFMR measurements reveal that as the net moment of the ensemble decreases, the strength of the spin-transfer torque increases relative to those of magnetic field torques. Our findings point to spin-transfer torque as an effective way to manipulate the state of nanomagnet ensembles at subnanosecond time scales.

Evidence of Pure Spin-Current Generated by Spin Pumping in Interface-Localized States in Hybrid Metal-Silicon-Metal Vertical Structures.

Due to the difficulty of growing high-quality semiconductors on ferromagnetic metals, the study of spin diffusion transport in Si was limited to lateral geometry devices. In this work, by using an ultrahigh-vacuum wafer-bonding technique, we have successfully fabricated metal-semiconductor-metal CoFeB/MgO/Si/Pt vertical structures. We hereby demonstrate pure spin-current injection and transport in the perpendicular current flow geometry over a distance larger than 2 µm in n-type Si at room temperature. In those experiments, a pure propagating spin current is generated via ferromagnetic resonance spin pumping and converted into a measurable voltage by using the inverse spin Hall effect occurring in the top Pt layer. A systematic study varying both Si and MgO thicknesses reveals the important role played by the localized states at the MgO-Si interface for the spin-current generation. Proximity effects involving indirect exchange interactions between the ferromagnet and the MgO-Si interface states appears to be a prerequisite to establishing the necessary out-of-equilibrium spin population in Si under the spin-pumping action.

Giant Spin Pumping and Inverse Spin Hall Effect in the Presence of Surface and Bulk Spin-Orbit Coupling of Topological Insulator Bi2Se3.

Three-dimensional (3D) topological insulators are known for their strong spin-orbit coupling (SOC) and the existence of spin-textured surface states that might be potentially exploited for "topological spintronics." Here, we use spin pumping and the inverse spin Hall effect to demonstrate successful spin injection at room temperature from a metallic ferromagnet (CoFeB) into the prototypical 3D topological insulator Bi2Se3. The spin pumping process, driven by the magnetization dynamics of the metallic ferromagnet, introduces a spin current into the topological insulator layer, resulting in a broadening of the ferromagnetic resonance (FMR) line width. Theoretical modeling of spin pumping through the surface of Bi2Se3, as well as of the measured angular dependence of spin-charge conversion signal, suggests that pumped spin current is first greatly enhanced by the surface SOC and then converted into a dc-voltage signal primarily by the inverse spin Hall effect due to SOC of the bulk of Bi2Se3. We find that the FMR line width broadens significantly (more than a factor of 5) and we deduce a spin Hall angle as large as 0.43 in the Bi2Se3 layer.

Simulation study of the Gilbert damping in Ni80Fe20/Nd bilayers: comparison with experiments.

We present an experimental and computational investigation the Neodymium thickness dependence of the effective damping constant (αeff) inNi80Fe20/Neodymium (Py/Nd) bilayers. The computational results show that the magnetic damping is strongly dependent on the thickness of Nd, which is in agreement with experimental data. Self consistent solutions of the spin accumulation model and the local magnetisation were used in the simulations. It was not possible to obtain agreement with experiment under the assumption of an enhanced damping in a single Py monolayer. Instead, it was found that the enhanced damping due to spin pumping needed to be spread across two monolayers of Py. This is suggested to arise from interface mixing. Subsequently, the temperature dependence of the effective damping was investigated. It is found that, with increasing temperature, the influence of thermally-induced spin fluctuations on magnetic damping becomes stronger with increasing Nd thickness.

Probing the Spin-Momentum Locking on Rashba Surfaces via Spin Current.

In this study, we investigate the spin-momentum locking phenomenon on Rashba states of antimony (Sb) films. Utilizing spin pumping in conjunction with an external charge current, we uncover the topological properties of Sb surface states. Our key finding is the precise manipulation of the direction and magnitude of the charge current generated by the inverse Rashba-Edelstein effect. This control is achieved through the dynamic interaction between out-of-equilibrium pumped spins and spin-momentum-locked flowing spins, which are perpendicular to the charge current. Our results highlight Sb as a promising material for both fundamental and applied spintronics research. The studied Sb nanostructures demonstrate potential for the development of low-power logic gates operating with currents in the microampere range, paving the way for advanced spintronic applications.

Direct and Inverse Spin Splitting Effects in Altermagnetic RuO2.

Recently, the altermagnetic materials with spin splitting effect (SSE), have drawn significant attention due to their potential to the flexible control of the spin polarization by the Néel vector. Here, the direct and inverse altermagnetic SSE (ASSE) in the (101)-oriented RuO2 film with the tilted Néel vector are reported. First, the spin torque along the x-, y-, and z-axis is detected from the spin torque-induced ferromagnetic resonance (ST-FMR), and the z-spin torque emerges when the electric current is along the [010] direction, showing the anisotropic spin splitting of RuO2. Further, the current-induced modulation of damping is used to quantify the damping-like torque efficiency (ξDL) in RuO2/Py, and an anisotropic ξDL is obtained and maximized for the current along the [010] direction, which increases with the reduction of the temperature, indicating the present of ASSE. Next, by way of spin pumping measurement, the inverse altermagnetic spin splitting effect (IASSE) is studied, which also shows a crystal direction-dependent anisotropic behavior and temperature-dependent behavior. This work gives a comprehensive study of the direct and inverse ASSE effects in the altermagnetic RuO2, inspiring future altermagnetic materials and devices with flexible control of spin polarization.

Enhancing Magnetic Damping under GaAs Band-Edge Photoexcitation in a Co2FeAl/n-GaAs Heterojunction.

The ultrafast manipulation of spin in ferromagnet-semiconductor (FM/SC) heterojunctions is a key issue for advancing spintronics, where magnetic damping and interfacial spin transport often define device efficiency. Leveraging selective optical excitation in semiconductors offers a unique approach to spin manipulation in FM/SC heterojunctions. Herein, we investigated the magnetic dynamics of a Co2FeAl/n-GaAs heterojunction using the time-resolved magneto-optical Kerr technique and observed the considerably enhanced magnetic damping of Co2FeAl when GaAs is photoexcited near its band edge. This enhancement is attributed to an enhanced spin-pumping effect facilitated by spin-dependent carrier tunneling and capture within the Co2FeAl layer. Moreover, circularly polarized light excites spin-polarized band-edge photocarriers, further impacting the magnetic damping of Co2FeAl through an additional optical spin-transfer torque on the magnetic moment of Co2FeAl. Our results provide a valuable reference for manipulating spin-pumping and interfacial spin transport in FM/SC heterojunctions, showcasing the advantage of optical control of semiconductor photocarriers for the ultrafast manipulation of magnetic dynamics and interfacial spin transfer.

Phase coupling of acoustic and optical modes in antiferromagnetic materials CrCl3.

In layered antiferromagnetic material CrCl3, due to the antiferromagnetic coupling between two magnetic sublattices, there are two antiferromagnetic resonance modes, called acoustic mode with in-phase precession and optical mode with out-of-phase precession. By using Landau-Lifshitz-Gilbert equation, we study the magnetization dynamics of the two sublattices in CrCl3. A coupling resonance mode appears at the coupling point when the acoustic and optical magnon modes are tuned by an applied magnetic field, which is called 'coupling mode'. In this paper, we present an explanation for the coupling of the acoustic and the optical mode. Our calculation shows that the coupling of the acoustic and optical mode is accomplished by change of the precession phase-difference between two magnetic sublattices.

Exploiting the Close-to-Dirac Point Shift of the Fermi Level in the Sb2Te3/Bi2Te3 Topological Insulator Heterostructure for Spin-Charge Conversion.

Properly tuning the Fermi level position in topological insulators is of vital importance to tailor their spin-polarized electronic transport and to improve the efficiency of any functional device based on them. Here, we report the full in situ metal organic chemical vapor deposition (MOCVD) and study of a highly crystalline Bi2Te3/Sb2Te3 topological insulator heterostructure on top of large area (4″) Si(111) substrates. The bottom Sb2Te3 layer serves as an ideal seed layer for the growth of highly crystalline Bi2Te3 on top, also inducing a remarkable shift of the Fermi level to place it very close to the Dirac point, as visualized by angle-resolved photoemission spectroscopy. To exploit such ideal topologically protected surface states, we fabricate the simple spin-charge converter Si(111)/Sb2Te3/Bi2Te3/Au/Co/Au and probe the spin-charge conversion (SCC) by spin pumping ferromagnetic resonance. A large SCC is measured at room temperature and is interpreted within the inverse Edelstein effect, thus resulting in a conversion efficiency of λIEEE ∼ 0.44 nm. Our results demonstrate the successful tuning of the surface Fermi level of Bi2Te3 when grown on top of Sb2Te3 with a full in situ MOCVD process, which is highly interesting in view of its future technology transfer.

Strongly Correlated Exciton-Magnetization System for Optical Spin Pumping in CrBr3 and CrI3 .

Ferromagnetism in van der Waals systems, preserved down to a monolayer limit, attracted attention to a class of materials with general composition CrX3 (X=I, Br, and Cl), which are treated now as canonical 2D ferromagnets. Their diverse magnetic properties, such as different easy axes or varying and controllable character of in-plane or interlayer ferromagnetic coupling, make them promising candidates for spintronic, photonic, optoelectronic, and other applications. Still, significantly different magneto-optical properties between the three materials have been presenting a challenging puzzle for researchers over the last few years. Herewith, it is demonstrated that despite similar structural and magnetic configurations, the coupling between excitons and magnetization is qualitatively different in CrBr3 and CrI3 films. Through a combination of the optical spin pumping experiments with the state-of-the-art theory describing bound excitonic states in the presence of magnetization, we concluded that the hole-magnetization coupling has the opposite sign in CrBr3 and CrI3 and also between the ground and excited exciton state. Consequently, efficient spin pumping capabilities are demonstrated in CrBr3 driven by magnetization via spin-dependent absorption, and the different origins of the magnetic hysteresis in CrBr3 and CrI3 are unraveled.