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 150 mΩ and a local spin readout signal of 7.8 Ω 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.

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.

Valence-state mixing and reduced magnetic moment inFe3-δGeTe2single crystals with varying Fe content probed by x-ray spectroscopy.

We present a spectroscopic study of the magnetic properties ofFe3-δGeTe2single crystals with varying Fe content, achieved by tuning the stoichiometry of the crystals. We carried out x-ray absorption spectroscopy and analyzed the x-ray circular magnetic dichroism spectra using the sum rules, to determine the orbital and spin magnetic moments of the materials. We find a clear reduction of the spin and orbital magnetic moment with increasing Fe deficiency. Magnetic susceptibility measurements show that the reduction in magnetization is accompanied by a reduced Curie temperature. Multiplet calculations reveal that the Fe2+state increasingly mixes with a higher valence state when the Fe deficiency is increased. This effect is correlated with the weakening of the magnetic moment. As single crystals are the base material for exfoliation processes, our results are relevant for the assembly of 2D magnetic heterostructures.

Unusual Dzyaloshinskii-Moriya Interaction in Graphene/Fe3GeTe2 Van der Waals Heterostructure.

Dzyaloshinskii-Moriya interaction (DMI) is shown to induce a topologically protected chiral spin texture in magnetic/nonmagnetic heterostructures. In the context of van der Waals spintronic devices, graphene emerges as an excellent candidate material. However, due to its negligible spin-orbit interaction, inducing DMI to stabilize topological spins when coupled to 3d-ferromagnets remains challenging. Here, it is demonstrated that, despite these challenges, a sizeable Rashba-type spin splitting followed by significant DMI is induced in graphene/Fe3GeTe2. This is made possible due to an interfacial electric field driven by charge asymmetry together with the broken inversion symmetry of the heterostructure. These findings reveal that the enhanced DMI energy parameter, resulting from a large effective electron mass in Fe3GeTe2, remarkably contributes to stabilizing non-collinear spins below the Curie temperature, overcoming the magnetic anisotropy energy. These results are supported by the topological Hall effect, which coexists with the non-trivial breakdown of Fermi liquid behavior, confirming the interplay between spins and non-trivial topology. This work paves the way toward the design and control of interface-driven skyrmion-based devices.

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.

2D Ferromagnetic M3GeTe2 (M = Ni/Fe) for Boosting Intermediates Adsorption toward Faster Water Oxidation.

In this work, 2D ferromagnetic M3GeTe2 (MGT, M = Ni/Fe) nanosheets with rich atomic Te vacancies (2D-MGTv) are demonstrated as efficient OER electrocatalyst via a general mechanical exfoliation strategy. X-ray absorption spectra (XAS) and scanning transmission electron microscope (STEM) results validate the dominant presence of metal-O moieties and rich Te vacancies, respectively. The formed Te vacancies are active for the adsorption of OH* and O* species while the metal-O moieties promote the O* and OOH* adsorption, contributing synergistically to the faster oxygen evolution kinetics. Consequently, 2D-Ni3GeTe2v exhibits superior OER activity with only 370 mV overpotential to reach the current density of 100 mA cm-2 and turnover frequency (TOF) value of 101.6 s-1 at the overpotential of 200 mV in alkaline media. Furthermore, a 2D-Ni3GeTe2v-based anion-exchange membrane (AEM) water electrolysis cell (1 cm2) delivers a current density of 1.02 and 1.32 A cm-2 at the voltage of 3 V feeding with 0.1 and 1 m KOH solution, respectively. The demonstrated metal-O coordination with abundant atomic vacancies for ferromagnetic M3GeTe2 and the easily extended preparation strategy would enlighten the rational design and fabrication of other ferromagnetic materials for wider electrocatalytic applications.

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.

Current-Controllable and Reversible Multi-Resistance-State Based on Domain Wall Number Transition in 2D Ferromagnet Fe3GeTe2.

Controlling the multi-state switching is significantly essential for the extensive utilization of 2D ferromagnet in magnetic racetrack memories, topological devices, and neuromorphic computing devices. The development of all-electric functional nanodevices with multi-state switching and a rapid reset remains challenging. Herein, to imitate the potentiation and depression process of biological synapses, a full-current strategy is unprecedently established by the controllable resistance-state switching originating from the spin configuration rearrangement by domain wall number modulation in Fe3GeTe2. In particular, a strong correlation is uncovered in the reduction of domain wall number with the corresponding resistance decreasing by in-situ Lorentz transmission electron microscopy. Interestingly, the magnetic state is reversed instantly to the multi-domain wall state under a single pulse current with a higher amplitude, attributed to the rapid thermal demagnetization by simulation. Based on the neuromorphic computing system with full-current-driven artificial Fe3GeTe2 synapses with multi-state switching, a high accuracy of ≈91% is achieved in the handwriting image recognition pattern. The results identify 2D ferromagnet as an intriguing candidate for future advanced neuromorphic spintronics.

Negative Photoconductivity of Fe3GeTe2 Crystal with Native Heterostructure for Ultraviolet to Terahertz Ultra-Broadband Photodetection.

Gaining insight into the photoelectric behavior of ferromagnetic materials is significant for comprehensively grasping their intrinsic properties and broadening future application fields. Here, through a specially designed Fe3GeTe2/O-Fe3GeTe2 heterostructure, first, the broad-spectrum negative photoconductivity phenomenon of ferromagnetic nodal line semimetal Fe3GeTe2 is reported that covers UV-vis-infrared-terahertz bands (355 nm to 3000 µm), promising to compensate for the inadequacies of traditional optoelectronic devices. The significant suppression of photoexcitation conductivity is revealed to arise from the semimetal/oxidation (sMO) interface-assisted dual-response mechanism, in which the electron excitation origins from the semiconductor photoconductivity effect in high-energy photon region, and semimetal topological band-transition in low-energy photon region. High responsivities ranging from 103 to 100 mA W-1 are acquired within ultraviolet-terahertz bands under ±0.1 V bias voltage at room temperature. Notably, the responsivity of 2.572 A W-1 at 3000 µm (0.1 THz) and the low noise equivalent power of 26 pW Hz-1/2 surpass most state-of-the-art mainstream terahertz detectors. This research provides a new perspective for revealing the photoelectric conversion properties of Fe3GeTe2 crystal and paves the way for the development of spin-optoelectronic devices.

Proximity-Induced Interfacial Room-Temperature Ferromagnetism in Semiconducting Fe3GeTe2.

The discoveries of two-dimensional ferromagnetism and magnetic semiconductors highly enrich the magnetic material family for constructing spin-based electronic devices, but with an acknowledged challenge that the Curie temperature (Tc) is usually far below room temperature. Many efforts such as voltage control and magnetic ion doping are currently underway to enhance the functional temperature, in which the involvement of additional electrodes or extra magnetic ions limits their application in practical devices. Here we demonstrate that the magnetic proximity, a robust effect but with elusive mechanisms, can induce room-temperature ferromagnetism at the interface between sputtered Pt and semiconducting Fe3GeTe2, both of which do not show ferromagnetism at 300 K. The independent electrical and magnetization measurements, structure analysis, and control samples with Ta highlighting the role of Pt confirm that the ferromagnetism with the Tc of above 400 K arises from the Fe3GeTe2/Pt interfaces, rather than Fe aggregation or other artificial effects. Moreover, contrary to conventional ferromagnet/Pt structures, the spin current generated by the Pt layer is enhanced more than two times at the Fe3GeTe2/Pt interfaces, indicating the potential applications of the unique proximity effect in building highly efficient spintronic devices. These results may pave a new avenue to create room-temperature functional spin devices based on low-Tc materials and provide clear evidence of magnetic proximity effects by using nonferromagnetic materials.

Nonlocal Spin Valves Based on Graphene/Fe3GeTe2 van der Waals Heterostructures.

With recent advances in two-dimensional (2D) ferromagnets with enhanced Curie temperatures, it is possible to develop all-2D spintronic devices with high-quality interfaces using 2D ferromagnets. In this study, we have successfully fabricated nonlocal spin valves with Fe3GeTe2 (FGT) as the spin source and detector and multilayer graphene as the spin transport channel. The nonlocal spin transport signal was found to strongly depend on temperature and disappear at a temperature below the Curie temperature of the FGT flakes, which stemmed from the temperature-dependent ferromagnetism of FGT. The spin injection efficiency was estimated to be about 1%, close to that of conventional nonlocal spin valves with transparent contacts between ferromagnetic electrodes and the graphene channel. In addition, the spin transport signal was found to depend on the direction of the magnetic field and the magnitude of the current, which was due to the strong perpendicular magnetic anisotropy of FGT and the thermal effect, respectively. Our results provide opportunities to extend the applications of van der Waals heterostructures in spintronic devices.

Seeding and Emergence of Composite Skyrmions in a van der Waals Magnet.

Topological charge plays a significant role in a range of physical systems. In particular, observations of real-space topological objects in magnetic materials have been largely limited to skyrmions - states with a unitary topological charge. Recently, more exotic states with varying topology, such as antiskyrmions, merons, or bimerons and 3D states such as skyrmion strings, chiral bobbers, and hopfions, have been experimentally reported. Along these lines, the realization of states with higher-order topology has the potential to open new avenues of research in topological magnetism and its spintronic applications. Here, real-space imaging of such spin textures, including skyrmion, skyrmionium, skyrmion bag, and skyrmion sack states, observed in exfoliated flakes of the van der Waals magnet Fe3-x GeTe2 (FGT) is reported. These composite skyrmions may emerge from seeded, loop-like states condensed into the stripe domain structure, demonstrating the possibility to realize spin textures with arbitrary integer topological charge within exfoliated flakes of 2D magnets. The general nature of the formation mechanism motivates the search for composite skyrmion states in both well-known and new magnetic materials, which may yet reveal an even richer spectrum of higher-order topological objects.

Selectively Controlled Ferromagnets by Electric Fields in van der Waals Ferromagnetic Heterojunctions.

Charge transfer plays a key role at the interfaces of heterostructures, which can affect electronic structures and ultimately the physical properties of the materials. However, charge transfer is difficult to manipulate externally once the interface is formed. The recently discovered van der Waals ferromagnets with atomically sharp interfaces provided a perfect platform for the electrical control of interfacial charge transfer. Here, we report magnetoresistance experiments revealing electrically tunable charge transfer in Fe3GeTe2/Cr2Ge2Te6/Fe3GeTe2 all-magnetic van der Waals heterostructures, which can be exploited to selectively modify the switching fields of the top or bottom Fe3GeTe2 electrodes. The directional charge transfer from metallic Fe3GeTe2 to semiconducting Cr2Ge2Te6 is revealed by first-principles calculations, which remarkably modifies the magnetic anisotropy energy of Fe3GeTe2, leading to the dramatically suppressed coercivity. The electrically selective control of magnetism demonstrated in this study could stimulate the development of spintronic devices based on van der Waals magnets.

Emergent, Non-Aging, Extendable, and Rechargeable Exchange Bias in 2D Fe3 GeTe2 Homostructures Induced by Moderate Pressuring.

As a crucial concept in magnetism and spintronics, exchange bias (ExB) measures the asymmetry in the hysteresis loop of a pinned ferromagnet (FM)/antiferromagnet (AFM) interface. Previous studies are mainly focused on FM/AFM heterostructures composed of conventional bulk materials, whose complex interfaces prohibit precise control and full understanding of the phenomenon. Here, the enabling power of 2D magnets is exploited to demonstrate the emergence, non-aging, extendability, and rechargeability of ExB in van der Waals Fe3 GeTe2 homostructures, upon moderate pressuring. The emergence of the ExB is attributed to a local stress-induced FM-to-AFM transition, as validated using first-principles calculations, and confirmed in magneto-optical Kerr effect and second harmonic generation measurements. It is also observed that, negligible ExB aging before the training effect suddenly takes place through avalanching, pronounced delay of the avalanche via timed pressure repetition (extendability), ExB recovery in the post-training sample upon refreshed pressuring (rechargeability), and demonstrate its versatile tunability. These striking findings offer unprecedented insights into the underlying principles of ExB and its training, with immense technological applications in sight.

2D Magnetic Semiconductor Fe3GeTe2 with Few and Single Layers with a Greatly Enhanced Intrinsic Exchange Bias by Liquid-Phase Exfoliation.

A 2D van der Waals (vdW) magnet can get rid of the constraints of lattice matching and compatibility and then create a variety of vdW heterostructures, which provides a opportunity for spintronic devices. However, the ability to reliably exfoliate large, high-quality vdW ferromagnetic Fe3GeTe2 (FGT) nanoflakes in scaled-up production is severely limited. Herein, an efficient and stable three-stage sonication-assisted liquid-phase exfoliation was developed for mass preparation of high-structural-integrity few- and single-layer FGT nanoflakes with a greatly enhanced intrinsic exchange bias. The three stages include slicing crystals, weakening interlayer vdW forces, and using ultrasonic cavitation. The highest yield of FGT nanoflakes is 22.3 wt % with single layers accounting for 6%. The size is controllable, and several micrometers, tens of micrometers, and a maximum of 103 µm are available. The 200 mg level output has overcome the limitations of mechanical exfoliation and molecular beam epitaxy in economically amplificated production. An intrinsic exchange bias is observed in the restacked nanoflakes due to the magnetic proximity on the interface of the FGT/natural surface oxide layer. The material reaches 578 Oe (2 K) and 2300 Oe after further oxidation, at least 250% higher than other precisely tailored vdW magnetic heterostructures. In addition, the unusual semiconductivity of the liquid-phase exfoliated FGT nanoflakes is reported. This work skillfully utilizes oxidation to enhance the potential of FGT for large-scale spintronics, optoelectronics, efficient data storage, and various extended applications, and it is beneficial for exfoliating other promising magnetic vdW materials.

Layer-Dependent Magnetic Domains in Atomically Thin Fe5GeTe2.

Magnetic domain formation in two-dimensional (2D) materials gives perspectives into the fundamental origins of 2D magnetism and also motivates the development of advanced spintronics devices. However, the characterization of magnetic domains in atomically thin van der Waals (vdW) flakes remains challenging. Here, we employ X-ray photoemission electron microscopy (XPEEM) to perform layer-resolved imaging of the domain structures in the itinerant vdW ferromagnet Fe5GeTe2 which shows near room temperature bulk ferromagnetism and a weak perpendicular magnetic anisotropy (PMA). In the bulk limit, we observe the well-known labyrinth-type domains. Thinner flakes, on the other hand, are characterized by increasingly fragmented domains. While PMA is a characteristic property of Fe5GeTe2, we observe a spin-reorientation transition with the spins canting in-plane for flakes thinner than six layers. Notably, a bubble phase emerges in four-layer flakes. This thickness dependence, which clearly deviates from the single-domain behavior observed in other 2D magnetic materials, demonstrates the exciting prospect of stabilizing complex spin textures in 2D vdW magnets at relatively high temperatures.

Magnetoresistance studies of two-dimensional Fe3GeTe2nano-flake.

The magneto-transport properties of two-dimensional (2D) Fe3GeTe2(FGT) nano-flakes are carefully investigated with the variation of the temperature and the direction of the applied magnetic field (B). Four magnetoresistance (MR) behavior are obtained at different temperatures withBparalleling the flake's surface, because of the competition between the merging of different domains, spin fluctuation, and the spin momentum flipping. Different from the reported negative MR of bulk FGT, 2D FGT shows a positive MR behavior with the increase ofBat a low temperature in a lowBrange, owning to the domination of the spin momentum flipping induced by the weakening of the coupling between different layers with the decrease of the thickness of the FGT flake. The angle-dependence of the FGT MR is also investigated and can be well explained by the competition mentioned above.

High-Quality Ferromagnet Fe3GeTe2 for High-Efficiency Electromagnetic Wave Absorption and Shielding with Wideband Radar Cross Section Reduction.

A high-quality Fe3GeTe2 single crystal with good electrical, magnetic, and electromagnetic wave absorption and shielding properties was prepared in a large quantity (10 g level) by solid-phase sintering and recrystallization method, which would promote its in-depth research and practical application. It has good room-temperature electrical properties with a mobility of 42 cm2/V·s, a sheet (bulk) carrier concentration of +1.64 × 1018 /cm2 (+3.28 × 1020 /cm3), and a conductivity of 2196.35 S/cm. Also, a Curie temperature of 238 K indicates the high magnetic transition temperature and a paramagnetic Curie temperature of 301 K shows the large ferromagnetic-paramagnetic transition zone induced by the residual short-range ferromagnetic domains. Particularly, Fe3GeTe2 is in a loosely packed state when used as a loss agent; the electromagnetic wave absorption with a reflection loss of -34.7 dB at 3.66 GHz under thin thickness was shown. Meanwhile, the absorption band can be effectively regulated by varying the thickness. Moreover, Fe3GeTe2 in a close-packed state exhibits terahertz shielding values of 75.1 and 103.2 dB at very thin thicknesses of 70 and 380 µm, and the average shielding value is higher than 47 dB, covering the entire bandwidth from 0.1 to 3.0 THz. Furthermore, by using Fe3GeTe2 as a patch, the wideband radar cross-section can be effectively reduced by up to 33 dBsm. Resultantly, Fe3GeTe2 will be a promising candidate in the electromagnetic protection field.

The Magnetic Genome of Two-Dimensional van der Waals Materials.

Magnetism in two-dimensional (2D) van der Waals (vdW) materials has recently emerged as one of the most promising areas in condensed matter research, with many exciting emerging properties and significant potential for applications ranging from topological magnonics to low-power spintronics, quantum computing, and optical communications. In the brief time after their discovery, 2D magnets have blossomed into a rich area for investigation, where fundamental concepts in magnetism are challenged by the behavior of spins that can develop at the single layer limit. However, much effort is still needed in multiple fronts before 2D magnets can be routinely used for practical implementations. In this comprehensive review, prominent authors with expertise in complementary fields of 2D magnetism (i.e., synthesis, device engineering, magneto-optics, imaging, transport, mechanics, spin excitations, and theory and simulations) have joined together to provide a genome of current knowledge and a guideline for future developments in 2D magnetic materials research.

Exchange Bias in Molecule/Fe3 GeTe2 van der Waals Heterostructures via Spinterface Effects.

The exfoliation of layered magnetic materials generates atomically thin flakes characterized by an ultrahigh surface sensitivity, which makes their magnetic properties tunable via external stimuli, such as electrostatic gating and proximity effects. Another powerful approach to engineer magnetic materials is molecular functionalization, generating hybrid interfaces with tailored magnetic interactions, called spinterfaces. However, spinterface effects have not yet been explored on layered magnetic materials. Here, the emergence of spinterface effects is demonstrated at the interface between flakes of the prototypical layered magnetic metal Fe3 GeTe2 and thin films of Co-phthalocyanine. Magnetotransport measurements show that the molecular layer induces a magnetic exchange bias in Fe3 GeTe2 , indicating that the unpaired spins in Co-phthalocyanine develop antiferromagnetic ordering and pin the magnetization reversal of Fe3 GeTe2 via magnetic proximity. The effect is strongest for a Fe3 GeTe2 thickness of 20 nm, for which the exchange bias field reaches -840 Oe at 10 K and is measurable up to ≈110 K. This value compares very favorably with previous exchange bias fields reported for Fe3 GeTe2 in all-inorganic van der Waals heterostructures, demonstrating the potential of molecular functionalization to tailor the magnetism of van der Waals layered materials.