Interfacial Spin Research Articles

Engineering exchange bias at the interface of self-polarized ultrathin ferroelectric BaTiO3 and ferromagnetic La0.67Sr0.33MnO3

We investigate the emergence and optimization of conventional exchange bias (EB) in ultrathin (<10 nm) ferroelectric (FE) BaTiO3 (BTO)/ferromagnetic (FM) La0.67Sr0.33MnO3 (LSMO) epitaxial bilayers without an antiferromagnetic (AFM) material. The EB originates from the electronic orbital reconstruction at the FE-FM interface due to the ferroelectric polarization. We achieve maximum EB of approximately 42 Oe with single-domain polarization in nine-unit-cell-thick BTO, setting the BTO thickness above the critical threshold for ferroelectricity yet below the thickness of strain relaxation and multidomain breakdown. Furthermore, the LSMO layer needs to be thick enough to sustain both the FM layer and polarization-induced AFM spin configuration at the LSMO/BTO interface, yet as thin as possible to enable the EB loop shift. The temperature, training, field, and thickness dependence of the EB confirm that the LSMO/BTO interface exhibits conventional EB despite its unconventional origin. Using x-ray magnetic circular dichroism, scanning transmission electron microscopy, and density-functional-theory calculations, we confirm that the macroscopic EB effect originates from the interfacial AFM spin configuration in LSMO driven by FE-induced -orbital modifications in interfacial Mn ions. Thus, we engineer strong interfacial EB coupling in artificial multiferroics without a conventional AFM material by controlling FE polarization, highlighting the potential for advanced spintronic applications. Published by the American Physical Society 2024

High Efficiency Non‐Doped Organic Light Emitting Diodes Based on Pure Organic Room Temperature Phosphorescence by High‐Lying Singlet Exciton Fission

AbstractHeavy‐metal‐free pure organic room temperature phosphorescence (ORTP) holds great potential in the field of organic optoelectronic devices owing to low economic cost, simple preparation techniques, and high exciton utilization. However, it is still filled with challenges in realizing high efficiency organic light‐emitting diodes (OLEDs) and exploring the internal physical mechanism based on these ORTP molecules. Here, a high‐performance OLED induced by an unexpected interfacial spin‐mixing process between the ORTP molecule and interlayers is demonstrated, and the high efficiency electroluminescence (EL) mechanism is studied through magneto–electroluminescence (MEL) and magneto–photoluminescence (MPL) measurements. The steady‐state and transient PL properties imply that the interfacial effect is related to a high‐lying singlet fission (HLSF) process in the ORTP molecule itself. Further, the HLSF process and the corresponding energy level position are confirmed by the incident wavelength‐ and temperature‐dependent PL spectra and the magnetic‐field‐dependent transient PL. Finally, by optimizing the interfacial material adjacent to the emissive layer to utilize this interfacial spin mixing effect, a high‐efficiency non‐doped ORTP‐OLED with external quantum efficiency of 16% and CIE coordinates of (0.27, 0.49) is developed. The proposed mechanism during the EL process will give insight to produce more efficient OLEDs based on ORTP materials in the future.

Coherent spin wave excitation with radio-frequency spin–orbit torque

Spin waves, collective perturbations of magnetic moments, are both fundamental probes for magnetic physics and promising candidates for energy-efficient signal processing and computation. Traditionally, coherent propagating spin waves have been generated by radio frequency (RF) inductive Oersted fields from current-carrying electrodes. An alternative mechanism, spin–orbit torque (SOT), offers more localized excitation through interfacial spin accumulation but has been mostly limited to DC to kHz frequencies. SOT driven by RF currents, with potentially enhanced pumping efficiency and unique spin dynamics, remains largely unexplored, especially in magnetic insulators. Here, we conduct a comprehensive theoretical and computational investigation into the generation of coherent spin waves via RF-SOT in the prototypical yttrium iron garnet. We characterize the excitation of forward volume, backward volume, and surface modes in both linear and nonlinear regimes, employing single and interdigitated electrode configurations. We reveal and explain several unique and surprising features of RF-SOT compared to inductive excitation, including higher efficiency, distinct mode selectivity, and directional symmetry, a ∼3π/4 phase offset, reduced anharmonic distortion in the nonlinear regime, and the absence of second harmonic generation. These insights position RF-SOT as a promising new mechanism for future magnonic and spintronic applications.

Role of Spin Transport on Ultrafast Spin Dynamics in Magnetic Weyl Semimetal (Co2MnGa)/Pt Heterostructures with High Spin‐Mixing Conductance

AbstractMagnetic Weyl semimetals are emerging as a new class of material systems for spintronics due to their intrinsic topological properties and the inherent interplay between topology and magnetism, giving rise to novel electronic states and spin‐orbital‐related effects. Here, ultrafast magnetization dynamics in the Weyl semimetal Heusler ferromagnet Co2MnGa is investigated, from femtosecond to nanosecond timescales, using time‐resolved magneto‐optical Kerr effect (TR‐MOKE) at room temperature. Ultrafast demagnetization and precessional dynamics corresponding to the Kittel and perpendicular standing spin‐wave (PSSW) modes of Co2MnGa, interfaced with Pt thin films of varying thickness, have been investigated. The exchange stiffness constant of Co2MnGa is determined, as well as detailed information about spin‐transport across the Co2MnGa/Pt interface. From the modulation of Gilbert damping of Co2MnGa with Pt thickness, a very high intrinsic spin‐mixing conductance, G↑↓ = 1.73 × 1016 cm−2 is extracted of the interface and the spin diffusion length of Pt is determined to be 2.9 ± 0.2 nm. The interfacial spin transparency is found to reach a sizeable value of ≈83%, in the perfect spin‐sink regime, suggesting the great potential of this heterostructure for spin‐orbitronics and devices relying on ultrafast magnetization dynamics.

Impact of orbital hybridization on spin-polarized electronic transport through Ni-MAPbI3 interfaces

The solution-processed methylammonium lead tri-iodine (MAPbI3), with long spin lifetimes and large spin diffusion lengths, has merit for developing stable perovskite spin valves (PeSV) with low saturation fields. By far, it remains challenging to avoid ill-defined ferromagnet-MAPbI3 interfaces during device fabrications using solution methods and to quantify the hybridized interfacial electronic and magnetic structures. Herein, an annealing-free method was developed for the fabrication of MAPbI3 based PeSV. In comparison to a thermally annealed device, an improved room temperature magnetoresistance (MR) was achieved. We found remarkable interfacial contributions to anisotropic magnetoresistance and MR. The first-principles calculation was further adopted to quantify the interfacial spin and orbital moments. Our results suggest that the orbital hybridization and the spin transfer are remarkable for the formation of the spin-dependent interfacial density of states. It consequently affects magnetic switching behaviors. This study holds an exceptionally important role for a deep understanding of the spin-polarized electronic transport through the Ni-MAPbI3 hybridized interface.

Evolution of static and dynamic magnetic properties of Re/Co/Pt and Pt/Co/Re trilayers with enhanced Dzyaloshinskii-Moriya interaction

The influence of Re layer insertion either at the bottom or top interface of epitaxially grown Pt/Co/Pt heterostructures on their static and dynamic magnetic properties is discussed in terms of their crystalline structure. Magnetic properties were studied as a function of both Re and Co layer thicknesses (dRe and dCo, respectively) in the matrix-like samples with a double-wedge structure, in which the layer thickness gradients were oriented orthogonally. The comprehensive investigations of the changes in coercivity, perpendicular magnetic anisotropy, spin reorientation transition, interfacial Dzyaloshinskii-Moriya interaction (iDMI) and spin wave damping are reported. Two different magnetic phases depending on the Co layer thickness with volume anisotropies (determined without demagnetization term) of KV∼0.25 (low) and KV∼0.75 MJ/m3 (high) were observed. The relation between these phases depends on the stack sequence and thickness of Re inserted layer. For dRe = 0.2 ÷ 0.7 nm deposited as the bottom interface, dCo induced transition at dtr ∼ 2 nm from low to high volume anisotropy phases was observed. Low and high volume anisotropy phases are associated to Co fcc and hcp structural phases. The insertion of half atomic layer of Re had no influence on surface anisotropy but significantly enhanced iDMI above 1 pJ/m and reduced spin wave damping.

Engineering of Co/MgO interface with combination of ultrathin heavy metal insertion and post-oxidation for voltage-controlled magnetic anisotropy effect

The voltage-controlled magnetic anisotropy (VCMA) effect in ferromagnet/insulator junctions provides an effective way to manipulate electron spins, which can form the basis of future magnetic memory technologies. Recent studies have revealed that the VCMA effect can be strongly tuned by a process of “interface engineering” exploiting ultrathin heavy metal layers and an electron depletion effect. To further decrease the numbers of electrons, chemical reactions, such as surface oxidation of ferromagnets, may also be an effective way to achieve this depletion. However, the knowledge of combined effect of heavy metal layers and oxidation is still lacking. Here, we demonstrate that dual interfacial engineering using an insertion of heavy metals (Pt or Re) and a post-oxidation process can have a remarkable effect on the perpendicular magnetic anisotropy and the VCMA effect. Interestingly, a strong enhancement of the perpendicular magnetic anisotropy is observed by dual interfacial engineering with Pt insertion, although it does not occur with Pt insertion or surface oxidation alone. Furthermore, even a sign reversal of the additional VCMA effect due to the ultrathin heavy metal layers is observed by utilizing dual interfacial engineering. These findings provide another degree of freedom for designing voltage-controlled spintronic devices and pave the way to interfacial spin–orbit engineering for the VCMA effect.

Magnon excitation-induced spin memory loss in epitaxial L10-FePt/MgO/L10-FePt magnetic tunnel junctions

This work investigates the interplay between interfacial spin–orbit coupling (SOC) and magnon excitation-induced spin memory loss in epitaxial L10-FePt/MgO/L10-FePt magnetic tunnel junctions, which is crucial for advancing spintronic technologies. By employing systematic temperature-dependent transport measurements and inelastic electron tunneling spectroscopy, our study reveals that interfacial SOC at the Pt-terminated FePt/MgO interface significantly enhances magnon excitation during electron tunneling. This process results in a pronounced loss of spin memory in the spin-polarized current, diminishing the tunnel magnetoresistance ratio. Our findings provide critical insights into the mechanisms of spin memory loss, offering directions for optimizing spintronic device performance in the context of pronounced SOC environments.

Contributions of interfacial spin–orbit coupling to magnetic and spintronic properties in AuPt/ferromagnet bilayers

We investigate the relationships between various magnetic and spintronic properties within AuPt/ferromagnet (FM) bilayers (FM = CoFe, CoFeB, Py, and Co). A linear correlation between the volume and surface magnetic anisotropies is identified, potentially influenced by the magnetoelastic effect. The FM thickness dependence of the magnetic damping indicates that spin-memory loss due to the interfacial spin–orbit coupling (ISOC) and spin pumping to the heavy-metal layer contribute little to the damping. Instead, a notable contribution from two magnon scattering to the damping is recognized in AuPt/(Co, CoFe, CoFeB) bilayers, possibly originating from a magnetic inhomogeneity due to the ISOC. In addition, in contrast to the magnetic damping, spin–orbit-torque efficiencies are unlikely related to the ISOC in AuPt/FM systems. This work offers valuable insights into the correlations among magnetic and spintronic parameters arising from the interfaces, ultimately aiding in the advancement of magnetic memory and information processing systems.

Identifying the Origin of Thermal Modulation of Exchange Bias in MnPS3/Fe3GeTe2 van der Waals Heterostructures.

The exchange bias phenomenon, inherent in exchange-coupled ferromagnetic and antiferromagnetic systems, has intrigued researchers for decades. Van der Waals materials, with their layered structures, offer an ideal platform for exploring exchange bias. However, effectively manipulating exchange bias in van der Waals heterostructures remains challenging. This study investigates the origin of exchange bias in MnPS3/Fe3GeTe2 van der Waals heterostructures, demonstrating a method to modulate nearly 1000% variation in magnitude through simple thermal cycling. Despite the compensated interfacial spin configuration of MnPS3, a substantial 170 mT exchange bias is observed at 5 K, one of the largest observed in van der Waals heterostructures. This significant exchange bias is linked to anomalous weak ferromagnetic ordering in MnPS3 below 40 K. The tunability of exchange bias during thermal cycling is attributed to the amorphization and changes in the van der Waals gap during field cooling. The findings highlight a robust and adjustable exchange bias in van der Waals heterostructures, presenting a straightforward method to enhance other interface-related spintronic phenomena for practical applications. Detailed interface analysis reveals atom migration between layers, forming amorphous regions on either side of the van der Waals gap, emphasizing the importance of precise interface characterization in these heterostructures.

The Role of Interfacial Interactions and Oxygen Vacancies in Tuning Magnetic Anisotropy in LaCrO3/LaMnO3 Heterostructures

AbstractThe interplay of lattice, electronic, and spin degrees of freedom at epitaxial complex oxide interfaces provides a route to tune their magnetic ground states. Unraveling the competing contributions is critical for tuning their functional properties. The relationship between magnetic ordering and magnetic anisotropy and the lattice symmetry, oxygen content, and film thickness in compressively strained LaMnO3 (LMO)/LaCrO3 (LCO) superlattices is investigated. Mn–O–Cr antiferromagnetic superexchange interactions across the heterointerface result in a net ferrimagnetic magnetic structure. Bulk magnetometry measurements reveal isotropic in‐plane magnetism for as‐grown oxygen‐deficient thin samples due to equal fractions of orthorhombic a+a‐c‐, and a‐a+c‐ twin domains. As the superlattice thickness is increased, in‐plane magnetic anisotropy emerges as the fraction of the a+a‐c‐ domain increases. On annealing in oxygen, the suppression of oxygen vacancies results in a contraction of the lattice volume, and an orthorhombic to rhombohedral transition leads to isotropic magnetism independent of the film thickness. The complex interactions are investigated using high‐resolution synchrotron diffraction and X‐ray absorption spectroscopy. These results highlight the role of the evolution of structural domains with film thickness, interfacial spin interactions, and oxygen‐vacancy‐induced structural phase transitions in tuning the magnetic properties of complex oxide heterostructures.

Spin-anomalous-Hall unidirectional magnetoresistance in light-metal/ferromagnetic-metal bilayers

Nonreciprocal magnetotransport is one of the central topics in spintronics because of its importance for electrically probing magnetic information. Among numerous electrical probes used to read magnetic orders, unidirectional magnetoresistance (UMR), characterized by sign changes upon reversal of either current or magnetization, is currently a matter of great interest and has been identified in various spin–orbit-coupled bilayer systems composed of an (anti)ferromagnetic layer and a nonmagnetic layer with strong spin Hall effect. A recent theoretical work predicts that a spin-anomalous-Hall (SAH) UMR in those metallic conducting bilayers can originate from the spin-anomalous-Hall effect of the ferromagnetic layer and the structural inversion asymmetry. However, this type of UMR has not been reported experimentally. Here, we give the experimental evidence of spin-anomalous-Hall UMR in the light-metal/ferromagnetic-metal Cu/Co bilayers, where the emergence of net nonequilibrium spin density is attributed to the interfacial spin leakage asymmetry due to the spin memory loss effect at the Cu/Co interface and multiple spin reflections. We also show a highly tunable UMR in the Cu/Co/CuOx trilayer by varying the Cu thickness, which is due to the competition between the orbital Rashba effect in Co/CuOx and the spin-anomalous-Hall effect in Cu/Co. Our work widens the material choice for UMR device applications and provides an alternative approach to detect in-plane magnetization without an external spin polarizer.

Thermal and Coherent Spin Pumping by Noncollinear Antiferromagnets.

Antiferromagnets attract much interest because of their potential for spintronic applications and open fundamental physics questions, but especially noncollinear antiferromagnets remain relatively unexplored. Here, we formulate the thermal and coherent pumping of spins in noncollinear antiferromagnets|normal metal bilayers. We find that the spin current polarization is a vector with components along both the Néel vector and net magnetic moment. The spin mixing conductance for the coherent spin pumping is a tensor with elements depending on the degree of noncollinearity and interface spin configuration. We explain the controversial sign problem of the antiferromagnetic spin Seebeck effect by interface effects and suggest that interface engineering may enhance the spin pumping efficiency.

Anchoring Atomically Precise Chiral Bismuth Oxido Nanoclusters on Gold: The Role of Amino Acid Linkers.

The adsorption of chiral molecules onto metallic surfaces triggers electron spin polarization at the interface, paving the way for applications in chiral opto-spintronics. However, the spin effects sensitively depend on the binding and ordering of the chiral species on surfaces. This study explores the adsorption of chiral thioether-functionalized atomically precise bismuth oxido nanoclusters (BiO-NCs) on gold (Au) surfaces, extending the conventional approach of using thiol-containing molecules and complexes to nanoclusters. Starting from the precursor [Bi38O45(NO3)20(dmso)28](NO3)4·4dmso (A), chiral BiO-NCs were synthesized by substituting the nitrates with N-(tert-butoxycarbonyl)-l-methionine (Boc-l-Met-O-) ligands to obtain [Bi38O45(Boc-l-Met-O)24] (2). The full exchange of nitrate by the Boc-l-methionine ligand was demonstrated by powder X-ray diffractograms, dynamic light scattering, electrospray ionization mass spectrometry, nuclear magnetic resonance, infrared, circular dichroism, and X-ray photoelectron spectroscopy. Compared to previously reported [Bi38O45(Boc-l-Phe-O)24(dmso)9] (1), BiO-NC 2 shows differences in the growth mode on a Au surface as revealed by scanning electron microscopy, wherefore a stronger binding of BiO-NC 2 is assumed. Anchoring of BiO-NC 2 to the Au surface through thioether groups induced a discernible change in the optical response of the Au surface analyzed by spectroscopic ellipsometry (SE). From the numerical modeling of the SE parameters, a layer thickness of ∼2 nm, corresponding to a monolayer of BiO-NC 2, was estimated for the samples prepared by dip coating. Thus, strong adsorption of BiO-NC 2 to the Au surface is concluded, which is an essential prerequisite for chiral-induced interface spin polarization.

Highly Efficient Spin Injection and Readout Across Van Der Waals Interface.

Spin injection, transport, and detection across the interface between a ferromagnet and a spin-carrying channel are crucial for energy-efficient spin logic devices. However, interfacial conductance mismatch, spin dephasing, and inefficient spin-to-charge conversion significantly reduce the efficiency of these processes. In this study, it is demonstrated that an all van der Waals heterostructure consisting of a ferromagnet (Fe3GeTe2) and Weyl semimetal enables a large spin readout efficiency. Specifically, a nonlocal spin readout signal of 150mΩ and a local spin readout signal of 7.8Ω is achieved, which reach the signal level useful for practical spintronic devices. The remarkable spin readout signal is attributed to suppressed spin dephasing channels at the vdW interfaces, long spin diffusion, and efficient charge-spin interconversion in Td-MoTe2. These findings highlight the potential of vdW heterostructures for spin Hall effect-enabled spin detection with high efficiency, opening up new possibilities for spin-orbit logic devices using vdW interfaces.

Emergent chiral spin textures in centrosymmetric iron garnet with spin alignment constraints

Chiral spin textures have emerged as a captivating class of topological matter. These intriguing structures harbor localized and topologically protected magnetic textures, rendering them promising candidates for novel spintronic applications. Here, the emergent chiral spin textures in an iron garnet with nanodisk configuration have been micromagnatically simulated based on the Landau-Lifshitz-Gilbert equation (LLG) of COMSOL Multiphysics. The modification of magnetic spin texture in the considered iron garnet has been controlled by introducing the interfacial Dzyaloshinskii-Moriya interaction (I-DMI) and spin alignment constraints as locally pinned spins and curvilinear defects at edges. These boundary conditions induced interesting chiral textures not commonly observed in such iron garnet due to its centrosymmetric crystal structure. The simulation results showed the presence of two distinct regions of spin texture: inside and outside the pinning boundary. By systematically varying the DMI strength (D) with the size of the pinning boundary (Rpin) and the number of defects (Ndef), the emerging chiral spin textures have been explored and reported, including the existence of ramified helical stripes, skyrmions, and skyrmions-like textures such as elongated skyrmions, chiral horseshoe domains, biskyrmions and target skyrmions (TSk) (2π-TSk and 3π-TSk). Also, it has been reported that various collapses occur in the final spin texture states, leading to the transition from one state to another when varying the values of Rpin and Ndef with D.

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.

Syntropic spin alignment at the interface between ferromagnetic and superconducting nitrides.

The magnetic correlations at the superconductor/ferromagnet (S/F) interfaces play a crucial role in realizing dissipation-less spin-based logic and memory technologies, such as triplet-supercurrent spin-valves and 'π' Josephson junctions. Here we report the observation of an induced large magnetic moment at high-quality nitride S/F interfaces. Using polarized neutron reflectometry and DC SQUID measurements, we quantitatively determined the magnetization profile of the S/F bilayer and confirmed that the induced magnetic moment in the adjacent superconductor only exists below T C. Interestingly, the direction of the induced moment in the superconductors was unexpectedly parallel to that in the ferromagnet, which contrasts with earlier findings in S/F heterostructures based on metals or oxides. First-principles calculations verified that the unusual interfacial spin texture observed in our study was caused by the Heisenberg direct exchange coupling with constant J∼4.28 meV through d-orbital overlapping and severe charge transfer across the interfaces. Our work establishes an incisive experimental probe for understanding the magnetic proximity behavior at S/F interfaces and provides a prototype epitaxial 'building block' for superconducting spintronics.

Interfacial magnetic spin Hall effect in van der Waals Fe3GeTe2/MoTe2 heterostructure

The spin Hall effect (SHE) allows efficient generation of spin polarization or spin current through charge current and plays a crucial role in the development of spintronics. While SHE typically occurs in non-magnetic materials and is time-reversal even, exploring time-reversal-odd (T-odd) SHE, which couples SHE to magnetization in ferromagnetic materials, offers a new charge-spin conversion mechanism with new functionalities. Here, we report the observation of giant T-odd SHE in Fe3GeTe2/MoTe2 van der Waals heterostructure, representing a previously unidentified interfacial magnetic spin Hall effect (interfacial-MSHE). Through rigorous symmetry analysis and theoretical calculations, we attribute the interfacial-MSHE to a symmetry-breaking induced spin current dipole at the vdW interface. Furthermore, we show that this linear effect can be used for implementing multiply-accumulate operations and binary convolutional neural networks with cascaded multi-terminal devices. Our findings uncover an interfacial T-odd charge-spin conversion mechanism with promising potential for energy-efficient in-memory computing.

Strong Anisotropic Order Parameters at All-Nitride Ferromagnet/Superconductor Interfaces

Proximity effects between superconductors and ferromagnets (SC/FM) hold paramount importance in comprehending the spin competition transpiring at their interfaces. This competition arises from the interplay between Cooper pairs and ferromagnetic exchange interactions. The proximity effects between transition metal nitrides (TMNs) are scarcely investigated due to the formidable challenges of fabricating high-quality SC/FM interfaces. We fabricated heterostructures comprising SC titanium nitride (TiN) and FM iron nitride (Fe3N) with precise chemical compositions and atomically well-defined interfaces. The magnetoresistance of Fe3N/TiN heterostructures shows a distinct magnetic anisotropy and strongly depends on the external perturbations. Moreover, the superconducting transition temperature T C and critical field of TiN experience notable suppression when proximity to Fe3N. We observe the intriguing competition of interfacial spin orientations near T C (∼ 1.25 K). These findings not only add a new materials system for investigating the interplay between superconductor and ferromagnets, but also potentially provide a building block for future research endeavors and applications in the realms of superconducting spintronic devices.