Manipulation of Exchange Bias in Two-Dimensional van der Waals Ferromagnet Near Room Temperature.

As a host for exchange bias (EB), van der Waals (vdW) magnetic materials have exhibited intriguing and distinct functionalities from conventional magnetic materials. The EB in most vdW systems is far below room temperature, which poses a challenge for practical applications. Here, by using Kerr microscopy, we demonstrate a record-high blocking temperature that approaches room temperature and a huge positive EB field that nears 2 kOe at 100 K in naturally oxidized two-dimensional (2D) vdW ferromagnetic Fe3GaTe2 nanoflakes. Moreover, we realized a reversible manipulation of both the presence/absence and positive/negative signs of EB via a training magnetic field without multiple field cooling processes. Thus, our study clearly reveals the robust, sizable, and sign-tunable EB in vdW magnetic materials up to near room temperature, thereby establishing Fe3GaTe2 as an emerging room-temperature-operating vdW material and paving the way for designing practical 2D spintronic devices.

Strain-Induced Robust Exchange Bias Effect in Epitaxial La0.7Sr0.3MnO3/LaFeO3 Bilayers.

The ground state of correlated electrons in complex oxide films can be controlled by applying epitaxial strain, offering the potential to produce unexpected phenomena applicable to modern spintronic devices. In this study, we demonstrate that substrate-induced strain strongly affects the coupling mode of interfacial magnetic moments in a ferromagnetic (FM)/antiferromagnetic (AFM) system. In an epitaxial bilayer comprising AFM LaFeO3 (LFO) and FM La0.7Sr0.3MnO3 (LSMO), samples grown on a LaAlO3 (LAO) substrate exhibit a larger exchange bias field than those grown on a SrTiO3 substrate. Our results indicate a transition in the alignment of magnetic moments from perpendicular to collinear due to the large compressive strain exerted by the LAO substrate. Collinear magnetic moments at the LSMO/LFO interface generate strong exchange coupling, leading to a considerable exchange bias effect. Thus, our findings provide a method for tailoring and manipulating the orientations of magnetic moments at the FM/AFM heterogeneous interface using strain engineering, thereby augmenting methods for exchange bias generation.

Asymmetric Manipulation of Perpendicular Exchange Bias and Programmable Spin Logical Cells by Spin-Orbit Torque in a Ferromagnet/Antiferromagnet System.

Antiferromagnets are competitive candidates for the next generation of spintronic devices owing to their superiority in small-scale and low-power-consumption devices. The electrical manipulation of the magnetization and exchange bias (EB) driven by spin-orbit torque (SOT) in ferromagnetic (FM)/antiferromagnetic (AFM) systems has become focused in spintronics. Here, the realization of a large perpendicular EB field in Co/IrMn and the effective manipulation of the magnetic moments of the magnetic Co layer and EB field by SOT in Pt/Co/IrMn system is reported. During the SOT-driven switching process, an asymmetrically manipulated state is observed. Current pulses with the same amplitude but opposite directions induce different magnetization states. Magneto-optical Kerr measurements reveal that this is due to the coexistence of stable and metastable antiferromagnetic domains in the AFM. Exploiting the asymmetric properties of these FM/AFM structures, five spin logic gates, namely AND, OR, NOR, NAND, and NOT, are realized in a single cell via SOT. This study provides an insight into the special ability of SOT on AFMs and also paves an avenue to construct the logic-in-memory and neuromorphic computing cells based on the AFM spintronic system.

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.

Comparative study on the magnetic properties of Fe-substituted Co2Sn1-xFexO4spinel oxides and its exchange bias effect.

Herein, we report the Fe-substituted Co2Sn1-xFexO4(0 ⩽ x ⩽ 0.4) inverse spinel's oxide using the solid-state reaction method. X-ray reveals the single-phase cubic structure with space group Fd3m. With increasing Fe in Co2Sn1-xFexO4spinel oxide, the transition temperature rise. The ac susceptibility at different frequencies also confirms a spin-glassy state at lower temperatures. The strong exchange bias effect appears in the sample having Fe substitution (x= 0.2) under the presence of constant temperature ∼10 K. The high-temperature susceptibility of Curie-Wise fitting shows that the system changes from antiferromagnetic exchange (x< 0.2) to ferromagnetic exchange (x> 0.2).

Zero-field magnetic skyrmions in exchange-biased ferromagnetic-antiferromagnetic bilayers.

We report on the stabilization of ferromagnetic skyrmions in zero external magnetic fields, in exchange-biased systems composed of ferromagnetic-antiferromagnetic (FM-AFM) bilayers. By performing atomistic spin dynamics simulations, we study cases of compensated, uncompensated, and partly uncompensated FM-AFM interfaces, and investigate the impact of important parameters such as temperature, inter-plane exchange interaction, Dzyaloshinskii-Moriya interaction, and magnetic anisotropy on the skyrmions appearance and stability. The model with an uncompensated FM-AFM interface leads to the stabilization of individual skyrmions and skyrmion lattices in the FM layer, caused by the effective field from the AFM instead of an external magnetic field. Similarly, in the case of a fully compensated FM-AFM interface, we show that FM skyrmions can be stabilized. We also demonstrate that accounting for interface roughness leads to stabilization of skyrmions both in compensated and uncompensated interface. Moreover, in bilayers with a rough interface, skyrmions in the FM layer are observed for a wide range of exchange interaction values through the FM-AFM interface, and the chirality of the skyrmions depends critically on the exchange interaction.

Even-Odd Layer-Dependent Exchange Bias Effect in MnBi2Te4 Chern Insulator Devices.

Magnetic topological materials with coexisting magnetism and nontrivial band structures exhibit many novel quantum phenomena, including the quantum anomalous Hall effect, the axion insulator state, and the Weyl semimetal phase. As a stoichiometric layered antiferromagnetic topological insulator, thin films of MnBi2Te4 show fascinating even-odd layer-dependent physics. In this work, we fabricate a series of thin-flake MnBi2Te4 devices using stencil masks and observe the Chern insulator state at high magnetic fields. Upon magnetic field training, a large exchange bias effect is observed in odd but not in even septuple layer (SL) devices. Through theoretical calculations, we attribute the even-odd layer-dependent exchange bias effect to the contrasting surface and bulk magnetic properties of MnBi2Te4 devices. Our findings reveal the microscopic magnetic configuration of MnBi2Te4 thin flakes and highlight the challenges in replicating the zero magnetic field quantum anomalous Hall effect in odd SL MnBi2Te4 devices.

Neuromorphic Computing with Emerging Antiferromagnetic Ordering in Spin-Orbit Torque Devices.

Field-free switching (FFS) and spin-orbit torque (SOT)-based neuromorphic characteristics were realized in a W/Pt/Co/NiO/Pt heterostructure with a perpendicular exchange bias (HEB) for brain-inspired neuromorphic computing (NC). Experimental results using NiO-based SOT devices guided the development of fully spin-based artificial synapses and sigmoidal neurons for implementation in a three-layer artificial neural network. This system achieved impressive accuracies of 91-96% when applied to the Modified National Institute of Standards and Technology (MNIST) image data set and 78.85-81.25% when applied to Fashion MNIST images, due presumably to the emergence of robust NiO antiferromagnetic (AFM) ordering. The emergence of AFM ordering favored the FFS with an enhanced HEB, which suppressed the memristivity and reduced the recognition accuracy. This indicates a trade-off between the requirements for solid-state memory and those required for brain-inspired NC devices. Nonetheless, our findings revealed opportunities by which the two technologies could be aligned via controllable exchange coupling.

Unraveling the Correlation between the Interface Structures and Tunable Magnetic Properties of La1-xSrxCoO3-δ/La1-xSrxMnO3-δ Bilayers Using Deep Learning Models.

Perovskite oxides are gaining significant attention for use in next-generation magnetic and ferroelectric devices due to their exceptional charge transport properties and the opportunity to tune the charge, spin, lattice, and orbital degrees of freedom. Interfaces between perovskite oxides, exemplified by La1-xSrxCoO3-δ/La1-xSrxMnO3-δ (LSCO/LSMO) bilayers, exhibit unconventional magnetic exchange switching behavior, offering a pathway for innovative designs in perovskite oxide-based devices. However, the precise atomic-level stoichiometric compositions and chemophysical properties of these interfaces remain elusive, hindering the establishment of surrogate design principles. We leverage first-principles simulations, evolutionary algorithms, and neural network searches with on-the-fly uncertainty quantification to design deep learning model ensembles to investigate over 50,000 LSCO/LSMO bilayer structures as a function of oxygen deficiency (δ) and strontium concentration (x). Structural analysis of the low-energy interface structures reveals that preferential segregation of oxygen vacancies toward the interfacial La0.7Sr0.3CoO3-δ layers causes distortion of the CoOx polyhedra and the emergence of magnetically active Co2+ ions. At the same time, an increase in the Sr concentration and a decrease in oxygen vacancies in the La0.7Sr0.3MnO3-δ layers tend to retain MnO6 octahedra and promote the formation of Mn4+ ions. Electronic structure analysis reveals that the nonuniform distributions of Sr ions and oxygen vacancies on both sides of the interface can alter the local magnetization at the interface, showing a transition from ferromagnetic (FM) to local antiferromagnetic (AFM) or ferrimagnetic regions. Therefore, the exotic properties of La1-xSrxCoO3-δ/La1-xSrxMnO3-δ are strongly coupled to the presence of hard/soft magnetic layers, as well as the FM to AFM transition at the interface, and can be tuned by changing the Sr concentration and oxygen partial pressure during growth. These insights provide valuable guidance for the precise design of perovskite oxide multilayers, enabling tailoring of their functional properties to meet specific requirements for various device applications.

Exchange Bias Induced by the Spin-Glass-Like State in a Te-Rich FeGeTe van der Waals Ferromagnet.

We have experimentally investigated the mechanism of the exchange bias in 2D van der Waals (vdW) ferromagnets by means of the anomalous Hall effect (AHE) together with the dynamical magnetization property. The temperature dependence of the AC susceptibility with its frequency response indicates a glassy transition of the magnetic property for the Te-rich FeGeTe vdW ferromagnet. We also found that the irreversible temperature dependence in the anomalous Hall voltage follows the de Almeida-Thouless line. Moreover, the freezing temperature of the spin-glass-like phase is found to correlate with the disappearance temperature of the exchange bias. These important signatures suggest that the emergence of magnetic exchange bias in the 2D van der Waals ferromagnets is induced by the presence of the spin-glass-like state in FeGeTe. The unprecedented insights gained from these findings shed light on the underlying principles governing exchange bias in vdW ferromagnets, contributing to the advancement of our understanding.

Asymmetric magnetoimpedance in exchange-biased systems.

Magnetic systems with competing anisotropies generally exhibit asymmetry between the maximum amplitudes of the right and left maxima in a magnetoimpedance curve. Small errors in positioning the samples at the experimental setup may also produce such asymmetry. In this work, we present a study on the sources of the asymmetry between magnetoimpedance peaks in systems that present the exchange bias phenomenon, by comparing a phenomenological model to experimental data. A set of samples with different repetitions of the NiFe/FeMn exchange-biased bilayer was used in this study. From the frequency evolution of the asymmetry, together with magnetization curves, we were able to identify the sources for the observed magnetoimpedance asymmetry found on our experimental data.

Size-induced exchange bias in single-phase CoO nanoparticles.

The tuning of exchange bias (EB) in nanoparticles has garnered significant attention due to its diverse range of applications. Here, we demonstrate EB in single-phase CoO nanoparticles, where two magnetic phases naturally emerge as the crystallite size decreases from 34.6 ± 0.8 to 10.8 ± 0.9 nm. The Néel temperature (TN) associated with antiferromagnetic ordering decreases monotonically with the reduction in crystallite size, highlighting the significant influence of size effects. The 34.6 nm nanoparticles exhibit magnetization irreversibility between zero-field cooled (ZFC) and field-cooled (FC) states belowTN. With further reduction in size this irreversibility appears well aboveTN, resulting in the absence of true paramagnetic regime which indicates the occurnace of an additional magnetic phase. The frequency-dependent ac-susceptibility in 10.8 nm nanoparticles suggests slow dynamics of disordered surface spins aboveTN, coinciding with the establishment of long-range order in the core. The thermoremanent magnetization (TRM) and iso-thermoremanent magnetization (IRM) curves suggest a core-shell structure: the core is antiferromagnetic, and the shell consists of disordered surface spins causing ferromagnetic interaction. Hence, the EB in these CoO nanoparticles results from the exchange coupling between an antiferromagnetic core and a disordered shell that exhibits unconventional surface spin characteristics.

Observation of Omnidirectional Exchange Bias at All-Antiferromagnetic Polycrystalline Heterointerface.

Due to promising functionalities that may dramatically enhance spintronics performance, antiferromagnets are the subject of intensive research for developing the next-generation active elements to replace ferromagnets. In particular, the recent experimental demonstration of tunneling magnetoresistance and electrical switching using chiral antiferromagnets has sparked expectations for the practical integration of antiferromagnetic materials into device architectures. To further develop the technology to manipulate the magnetic anisotropies in all-antiferromagnetic devices, it is essential to realize exchange bias through the interface between antiferromagnetic multilayers. Here, the first observation on the omnidirectional exchange bias at an all-antiferromagnetic polycrystalline heterointerface is reported. This experiment demonstrates that the interfacial energy causing the exchange bias between the chiral-antiferromagnet Mn3Sn/collinear-antiferromagnet MnN layers is comparable to those found at the conventional ferromagnet/antiferromagnet interface at room temperature. In sharp contrast with previous reports using ferromagnets, the magnetic field control of the unidirectional anisotropy is found to be omnidirectional due to the absence of the shape anisotropy in the antiferromagnetic multilayer. The realization of the omnidirectional exchange bias at the interface between polycrystalline antiferromagnets on amorphous templates, highly compatible with existing Si-based devices, paves the way for developing ultra-low power and ultra-high speed memory devices based on antiferromagnets.

Electrical-Controllable Antiferromagnet-Based Tunnel Junction.

An electrical-controllable antiferromagnet tunnel junction is a key goal in spintronics, holding immense promise for ultradense and ultrastable antiferromagnetic memory with high processing speed for modern information technology. Here, we have advanced toward this goal by achieving an electrical-controllable antiferromagnet-based tunnel junction of Pt/Co/Pt/Co/IrMn/MgO/Pt. The exchange coupling between antiferromagnetic IrMn and Co/Pt perpendicular magnetic multilayers results in the formation of an interfacial exchange bias and exchange spring in IrMn. Encoding information states "0" and "1" is realized through the exchange spring in IrMn, which can be electrically written by spin-orbit torque switching with high cyclability and electrically read by antiferromagnetic tunneling anisotropic magnetoresistance. Combining spin-orbit torque switching of both exchange spring and exchange bias, a 16 Boolean logic operation is successfully demonstrated. With both memory and logic functionalities integrated into our electrically controllable antiferromagnetic-based tunnel junction, we chart the course toward high-performance antiferromagnetic logic-in-memory.

Harnessing Van der Waals CrPS4 and Surface Oxides for Nonmonotonic Preset Field Induced Exchange Bias in Fe3GeTe2.

Two-dimensional van der Waals (vdW) heterostructures are an attractive platform for studying exchange bias due to their defect-free and atomically flat interfaces. Chromium thiophosphate (CrPS4), an antiferromagnetic material, possesses uncompensated magnetic spins in a single layer, rendering it a promising candidate for exploring exchange bias phenomena. Recent findings have highlighted that naturally oxidized vdW ferromagnetic Fe3GeTe2 exhibits exchange bias, attributed to the antiferromagnetic coupling of its ultrathin surface oxide layer (O-FGT) with the underlying unoxidized Fe3GeTe2. Anomalous Hall measurements are employed to scrutinize the exchange bias within the CrPS4/(O-FGT)/Fe3GeTe2 heterostructure. This analysis takes into account the contributions from both the perfectly uncompensated interfacial CrPS4 layer and the interfacial oxide layer. Intriguingly, a distinct and nonmonotonic exchange bias trend is observed as a function of temperature below 140 K. The occurrence of exchange bias induced by a "preset field" implies that the prevailing phase in the polycrystalline surface oxide is ferrimagnetic Fe3O4. Moreover, the exchange bias induced by the ferrimagnetic Fe3O4 is significantly modulated by the presence of the van der Waals antiferromagnetic CrPS4 layer, forming a heterostructure, along with additional iron oxide phases within the oxide layer. These findings underscore the intricate and complex nature of exchange bias in van der Waals heterostructures, highlighting their potential for tailored manipulation and control.

Single-Shot Laser-Induced Switching of an Exchange Biased Antiferromagnet.

Ultrafast manipulation of magnetic order has challenged the understanding of the fundamental and dynamic properties of magnetic materials. So far single-shot magnetic switching has been limited to ferrimagnetic alloys, multilayers, and designed ferromagnetic (FM) heterostructures. In FM/antiferromagnetic (AFM) bilayers, exchange bias (He) arises from the interfacial exchange coupling between the two layers and reflects the microscopic orientation of the antiferromagnet. Here the possibility of single-shot switching of the antiferromagnet (change of the sign and amplitude of He) with a single femtosecond laser pulse in IrMn/CoGd bilayers is demonstrated. The manipulation is demonstrated in a wide range of fluences for different layer thicknesses and compositions. Atomistic simulations predict ultrafast switching and recovery of the AFM magnetization on a timescale of 2 ps. The results provide the fastest and the most energy-efficient method to set the exchange bias and pave the way to potential applications for ultrafast spintronic devices.

Exchange Bias Modulated by Antiferromagnetic Spin-Flop Transition in 2D Van der Waals Heterostructures.

Exchange bias is extensively studied and widely utilized in spintronic devices, such as spin valves and magnetic tunnel junctions. 2D van der Waals (vdW) magnets, with high-quality interfaces in heterostructures, provide an excellent platform for investigating the exchange bias effect. To date, intrinsic modulation of exchange bias, for instance, via precise manipulation of the magnetic phases of the antiferromagnetic layer, is yet to be fully reached, owing partly to the large exchange fields of traditional bulk antiferromagnets. Herein, motivated by the low-field spin-flop transition of a 2D antiferromagnet, CrPS4, exchange bias is explored by modulating the antiferromagnetic spin-flop phase transition in all-vdW magnetic heterostructures. The results demonstrate that undergoing the spin-flop transition during the field cooling process, the A-type antiferromagnetic ground state of CrPS4 turns into a canted antiferromagnetic one, therefore, it reduces the interfacial magnetic coupling and suppresses the exchange bias. Via conducting different cooling fields, one can select the exchange bias effect switching among the "ON", "depressed", and "OFF" states determined by the spin flop of CrPS4. This work provides an approach to intrinsically modulate the exchange bias in all-vdW heterostructures and paves new avenues to design and manipulate 2D spintronic devices.

Nanoscale Magnetic Arrays through Block Copolymer Templating of Polyoxometalates.

Magnetic nanoarrays promise to enable new energy-efficient computations based on spintronics or magnonics. In this work, we present a block copolymer-assisted strategy for fabricating ordered magnetic nanostructures on silicon and permalloy substrates. Block copolymer micelle-like structures were used as a template in which polyoxometalate (POM) clusters could assemble in an opal-like structure. A combination of microscopy and scattering techniques was used to confirm the structural and organizational features of the fabricated materials. The magnetic properties of these materials were investigated by polarized neutron reflectometry, nuclear magnetic resonance, and magnetometry measurements. The data show that a magnetic structural design was achieved and that a thin layer of patterned POMs strongly influenced an underlying permalloy layer. This work demonstrates that the bottom-up pathway is a potentially viable method for patterning magnetic substrates on a sub-100 nm scale, toward the magnetic nanostructures needed for spintronic or magnonic crystal devices.

A Spin Valve-Based Rhombus-Shaped Micro-Object Implementing a Full Wheatstone Bridge.

Spin valves with a synthetic antiferromagnet were fabricated via magnetron sputtering. It was shown that the fabricated spin valve layers had a perfect microstructure and smooth interfaces, and therefore, an RKKY interaction dominated in the coupling of the ferromagnetic layers separated by a copper spacer. Rhombus-shaped micro-objects were fabricated from a single spin valve film. The thermomagnetic treatment procedure was found to form unidirectional anisotropy in the micro-object such that the values of the exchange bias fields in the rhombus' nonparallel sides were opposite in sign. For the CoFeNi/Ru/CoFeNi synthetic antiferromagnet, we determined the differences between the ferromagnetic layer thicknesses at which the thermomagnetic treatment formed the same exchange bias all over each rhombus' side. We also fabricated a sensor element in which each side of the rhombus was the shoulder of a Wheatstone bridge. After the thermomagnetic treatment procedure, each shoulder worked as an active magnetosensitive element, enabling the device to operate as a full Wheatstone bridge. The sensor output exhibited a step shape, high sensitivity to field changes, and significant magnetic hysteresis. Such characteristics are suitable for switching devices.

Magnetic Properties and THz Emission from Co/CoO/Pt and Ni/NiO/Pt Trilayers.

THz radiation emitted by ferromagnetic/non-magnetic bilayers is a new emergent field in ultra-fast spin physics phenomena with a lot of potential for technological applications in the terahertz (THz) region of the electromagnetic spectrum. The role of antiferromagnetic layers in the THz emission process is being heavily investigated at the moment. In this work, we fabricate trilayers in the form of Co/CoO/Pt and Ni/NiO/Pt with the aim of studying the magnetic properties and probing the role of very thin antiferromagnetic interlayers like NiO and CoO in transporting ultrafast spin current. First, we reveal the static magnetic properties of the samples by using temperature-dependent Squid magnetometry and then we quantify the dynamic properties with the help of ferromagnetic resonance spectroscopy. We show magnetization reversal that has large exchange bias values and we extract enhanced damping values for the trilayers. THz time-domain spectroscopy examines the influence of the antiferromagnetic interlayer in the THz emission, showing that the NiO interlayer in particular is able to transport spin current.