Epitaxial Growth of Large-Scale 2D CrTe2 Films on Amorphous Silicon Wafers With Low Thermal Budget.

2D van der Waals (vdW) magnets open landmark horizons in the development of innovative spintronic device architectures. However, their fabrication with large scale poses challenges due to high synthesis temperatures (>500 °C) and difficulties in integrating them with standard complementary metal-oxide semiconductor (CMOS) technology on amorphous substrates such as silicon oxide (SiO2 ) and silicon nitride (SiNx ). Here, a seeded growth technique for crystallizing CrTe2 films on amorphous SiNx /Si and SiO2 /Si substrates with a low thermal budget is presented. This fabrication process optimizes large-scale, granular atomic layers on amorphous substrates, yielding a substantial coercivity of 11.5 kilo-oersted, attributed to weak intergranular exchange coupling. Field-driven Néel-type stripe domain dynamics explain the amplified coercivity. Moreover, the granular CrTe2 devices on Si wafers display significantly enhanced magnetoresistance, more than doubling that of single-crystalline counterparts. Current-assisted magnetization switching, enabled by a substantial spin-orbit torque with a large spin Hall angle (85) and spin Hall conductivity (1.02 × 107 ℏ/2e Ω⁻¹ m⁻¹), is also demonstrated. These observations underscore the proficiency in manipulating crystallinity within integrated 2D magnetic films on Si wafers, paving the way for large-scale batch manufacturing of practical magnetoelectronic and spintronic devices, heralding a new era of technological innovation.

Topological Spin Textures in an Insulating van der Waals Ferromagnet.

Generation and control of topological spin textures constitutes one of the most exciting challenges of modern spintronics given their potential applications in information storage technologies. Of particular interest are magnetic insulators, which due to low damping, absence of Joule heating and reduced dissipation can provide energy-efficient spin-textures platform. Here, it is demonstrated that the interplay between sample thickness, external magnetic fields, and optical excitations can generate a prolific paramount of spin textures, and their coexistence in insulating CrBr3 van der Waals (vdW) ferromagnets. Using high-resolution magnetic force microscopy and large-scale micromagnetic simulation methods, the existence of a large region in T-B phase diagram is demonstrated where different stripe domains, skyrmion crystals, and magnetic domains exist and can be intrinsically selected or transformed to each-other via a phase-switch mechanism. Lorentz transmission electron microscopy unveils the mixed chirality of the magnetic textures that are of Bloch-type at given conditions but can be further manipulated into Néel-type or hybrid-type via thickness-engineering. The topological phase transformation between the different magnetic objects can be further inspected by standard photoluminescence optical probes resolved by circular polarization indicative of an existence of exciton-skyrmion coupling mechanism. The findings identify vdW magnetic insulators as a promising framework of materials for the manipulation and generation of highly ordered skyrmion lattices relevant for device integration at the atomic level.

Writing and Detecting Topological Charges in Exfoliated Fe5-xGeTe2.

Fe5-xGeTe2 is a promising two-dimensional (2D) van der Waals (vdW) magnet for practical applications, given its magnetic properties. These include Curie temperatures above room temperature, and topological spin textures─TST (both merons and skyrmions), responsible for a pronounced anomalous Hall effect (AHE) and its topological counterpart (THE), which can be harvested for spintronics. Here, we show that both the AHE and THE can be amplified considerably by just adjusting the thickness of exfoliated Fe5-xGeTe2, with THE becoming observable even in zero magnetic field due to a field-induced unbalance in topological charges. Using a complementary suite of techniques, including electronic transport, Lorentz transmission electron microscopy, and micromagnetic simulations, we reveal the emergence of substantial coercive fields upon exfoliation, which are absent in the bulk, implying thickness-dependent magnetic interactions that affect the TST. We detected a "magic" thickness t ≈ 30 nm where the formation of TST is maximized, inducing large magnitudes for the topological charge density (∼6.45 × 1020 cm-2), and the concomitant anomalous (ρxyA,max ≃22.6 µΩ cm) and topological (ρxyu,T 1≃5 µΩ cm) Hall resistivities at T ≈ 120 K. These values for ρxyA,max and ρxyu,T are higher than those found in magnetic topological insulators and, so far, the largest reported for 2D magnets. The hitherto unobserved THE under zero magnetic field could provide a platform for the writing and electrical detection of TST aiming at energy-efficient devices based on vdW ferromagnets.

Multistep magnetization switching in orthogonally twisted ferromagnetic monolayers.

The advent of twist engineering in two-dimensional crystals enables the design of van der Waals heterostructures with emergent properties. In the case of magnets, this approach can afford artificial antiferromagnets with tailored spin arrangements. Here we fabricate an orthogonally twisted bilayer by twisting two CrSBr ferromagnetic monolayers with an easy-axis in-plane spin anisotropy by 90°. The magnetotransport properties reveal multistep magnetization switching with a magnetic hysteresis opening, which is absent in the pristine case. By tuning the magnetic field, we modulate the remanent state and coercivity and select between hysteretic and non-hysteretic magnetoresistance scenarios. This complexity pinpoints spin anisotropy as a key aspect in twisted magnetic superlattices. Our results highlight control over the magnetic properties in van der Waals heterostructures, leading to a variety of field-induced phenomena and opening a fruitful playground for creating desired magnetic symmetries and manipulating non-collinear magnetic configurations.

Magnetic Imaging and Domain Nucleation in CrSBr Down to the 2D Limit.

Recent advancements in 2D materials have revealed the potential of van der Waals magnets, and specifically of their magnetic anisotropy that allows applications down to the 2D limit. Among these materials, CrSBr has emerged as a promising candidate, because its intriguing magnetic and electronic properties have appeal for both fundamental and applied research in spintronics or magnonics. In this work, nano-SQUID-on-tip (SOT) microscopy is used to obtain direct magnetic imaging of CrSBr flakes with thicknesses ranging from monolayer (N = 1) to few-layer (N = 5). The ferromagnetic order is preserved down to the monolayer, while the antiferromagnetic coupling of the layers starts from the bilayer case. For odd layers, at zero applied magnetic field, the stray field resulting from the uncompensated layer is directly imaged. The progressive spin reorientation along the out-of-plane direction (hard axis) is also measured with a finite applied magnetic field, allowing evaluation of the anisotropy constant, which remains stable down to the monolayer and is close to the bulk value. Finally, by selecting the applied magnetic field protocol, the formation of Néel magnetic domain walls is observed down to the single-layer limit.

Anomalous isotope effect on mechanical properties of single atomic layer Boron Nitride.

The ideal mechanical properties and behaviors of materials without the influence of defects are of great fundamental and engineering significance but considered inaccessible. Here, we use single-atom-thin isotopically pure hexagonal boron nitride (hBN) to demonstrate that two-dimensional (2D) materials offer us close-to ideal experimental platforms to study intrinsic mechanical phenomena. The highly delicate isotope effect on the mechanical properties of monolayer hBN is directly measured by indentation: lighter 10B gives rise to higher elasticity and strength than heavier 11B. This anomalous isotope effect establishes that the intrinsic mechanical properties without the effect of defects could be measured, and the so-called ultrafine and normally neglected isotopic perturbation in nuclear charge distribution sometimes plays a more critical role than the isotopic mass effect in the mechanical and other physical properties of materials.

Probing spin dynamics of ultra-thin van der Waals magnets via photon-magnon coupling.

Layered van der Waals (vdW) magnets can maintain a magnetic order even down to the single-layer regime and hold promise for integrated spintronic devices. While the magnetic ground state of vdW magnets was extensively studied, key parameters of spin dynamics, like the Gilbert damping, crucial for designing ultra-fast spintronic devices, remains largely unexplored. Despite recent studies by optical excitation and detection, achieving spin wave control with microwaves is highly desirable, as modern integrated information technologies predominantly are operated with these. The intrinsically small numbers of spins, however, poses a major challenge to this. Here, we present a hybrid approach to detect spin dynamics mediated by photon-magnon coupling between high-Q superconducting resonators and ultra-thin flakes of Cr2Ge2Te6 (CGT) as thin as 11 nm. We test and benchmark our technique with 23 individual CGT flakes and extract an upper limit for the Gilbert damping parameter. These results are crucial in designing on-chip integrated circuits using vdW magnets and offer prospects for probing spin dynamics of monolayer vdW magnets.

Laser-induced topological spin switching in a 2D van der Waals magnet.

Two-dimensional (2D) van der Waals (vdW) magnets represent one of the most promising horizons for energy-efficient spintronic applications because their broad range of electronic, magnetic and topological properties. However, little is known about the interplay between light and spin properties in vdW layers. Here we show that ultrafast laser excitation can not only generate different type of spin textures in CrGeTe3 vdW magnets but also induce a reversible transformation between them in a topological toggle switch mechanism. Our atomistic spin dynamics simulations and wide-field Kerr microscopy measurements show that different textures can be generated via high-intense laser pulses within the picosecond regime. The phase transformation between the different topological spin textures is obtained as additional laser pulses are applied to the system where the polarisation and final state of the spins can be controlled by external magnetic fields. Our results indicate laser-driven spin textures on 2D magnets as a pathway towards reconfigurable topological architectures at the atomistic level.

Coexistence of Merons with Skyrmions in the Centrosymmetric Van Der Waals Ferromagnet Fe5- x GeTe2.

Fe5- x GeTe2 is a centrosymmetric, layered van der Waals (vdW) ferromagnet that displays Curie temperatures Tc (270-330 K) that are within the useful range for spintronic applications. However, little is known about the interplay between its topological spin textures (e.g., merons, skyrmions) with technologically relevant transport properties such as the topological Hall effect (THE) or topological thermal transport. Here, via high-resolution Lorentz transmission electron microscopy, it is shown that merons and anti-meron pairs coexist with Néel skyrmions in Fe5- x GeTe2 over a wide range of temperatures and probe their effects on thermal and electrical transport. A THE is detected, even at room T, that senses merons at higher T's, as well as their coexistence with skyrmions as T is lowered, indicating an on-demand thermally driven formation of either type of spin texture. Remarkably, an unconventional THE is also observed in absence of Lorentz force, and it is attributed to the interaction between charge carriers and magnetic field-induced chiral spin textures. These results expose Fe5-x GeTe2 as a promising candidate for the development of applications in skyrmionics/meronics due to the interplay between distinct but coexisting topological magnetic textures and unconventional transport of charge/heat carriers.

Breaking through the Mermin-Wagner limit in 2D van der Waals magnets.

The Mermin-Wagner theorem states that long-range magnetic order does not exist in one- (1D) or two-dimensional (2D) isotropic magnets with short-ranged interactions. Here we show that in finite-size 2D van der Waals magnets typically found in lab setups (within millimetres), short-range interactions can be large enough to allow the stabilisation of magnetic order at finite temperatures without any magnetic anisotropy. We demonstrate that magnetic ordering can be created in 2D flakes independent of the lattice symmetry due to the intrinsic nature of the spin exchange interactions and finite-size effects. Surprisingly we find that the crossover temperature, where the intrinsic magnetisation changes from superparamagnetic to a completely disordered paramagnetic regime, is weakly dependent on the system length, requiring giant sizes (e.g., of the order of the observable universe ~ 1026 m) to observe the vanishing of the magnetic order as expected from the Mermin-Wagner theorem. Our findings indicate exchange interactions as the main ingredient for 2D magnetism.

All-optical control of spin in a 2D van der Waals magnet.

Two-dimensional (2D) van der Waals magnets provide new opportunities for control of magnetism at the nanometre scale via mechanisms such as strain, voltage and the photovoltaic effect. Ultrafast laser pulses promise the fastest and most energy efficient means of manipulating electron spin and can be utilized for information storage. However, little is known about how laser pulses influence the spins in 2D magnets. Here we demonstrate laser-induced magnetic domain formation and all-optical switching in the recently discovered 2D van der Waals ferromagnet CrI3. While the magnetism of bare CrI3 layers can be manipulated with single laser pulses through thermal demagnetization processes, all-optical switching is achieved in nanostructures that combine ultrathin CrI3 with a monolayer of WSe2. The out-of-plane magnetization is switched with multiple femtosecond pulses of either circular or linear polarization, while single pulses result in less reproducible and partial switching. Our results imply that spin-dependent interfacial charge transfer between the WSe2 and CrI3 is the underpinning mechanism for the switching, paving the way towards ultrafast optical control of 2D van der Waals magnets for future photomagnetic recording and device technology.

Thickness- and Twist-Angle-Dependent Interlayer Excitons in Metal Monochalcogenide Heterostructures.

Interlayer excitons, or bound electron-hole pairs whose constituent quasiparticles are located in distinct stacked semiconducting layers, are being intensively studied in heterobilayers of two-dimensional semiconductors. They owe their existence to an intrinsic type-II band alignment between both layers that convert these into p-n junctions. Here, we unveil a pronounced interlayer exciton (IX) in heterobilayers of metal monochalcogenides, namely, γ-InSe on ε-GaSe, whose pronounced emission is adjustable just by varying their thicknesses given their number of layers dependent direct band gaps. Time-dependent photoluminescense spectroscopy unveils considerably longer interlayer exciton lifetimes with respect to intralayer ones, thus confirming their nature. The linear Stark effect yields a bound electron-hole pair whose separation d is just (3.6 ± 0.1) Å with d being very close to dSe = 3.4 Å which is the calculated interfacial Se separation. The envelope of IX is twist-angle-dependent and describable by superimposed emissions that are nearly equally spaced in energy, as if quantized due to localization induced by the small moiré periodicity. These heterostacks are characterized by extremely flat interfacial valence bands making them prime candidates for the observation of magnetism or other correlated electronic phases upon carrier doping.

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.

A Chirality-Based Quantum Leap.

There is increasing interest in the study of chiral degrees of freedom occurring in matter and in electromagnetic fields. Opportunities in quantum sciences will likely exploit two main areas that are the focus of this Review: (1) recent observations of the chiral-induced spin selectivity (CISS) effect in chiral molecules and engineered nanomaterials and (2) rapidly evolving nanophotonic strategies designed to amplify chiral light-matter interactions. On the one hand, the CISS effect underpins the observation that charge transport through nanoscopic chiral structures favors a particular electronic spin orientation, resulting in large room-temperature spin polarizations. Observations of the CISS effect suggest opportunities for spin control and for the design and fabrication of room-temperature quantum devices from the bottom up, with atomic-scale precision and molecular modularity. On the other hand, chiral-optical effects that depend on both spin- and orbital-angular momentum of photons could offer key advantages in all-optical and quantum information technologies. In particular, amplification of these chiral light-matter interactions using rationally designed plasmonic and dielectric nanomaterials provide approaches to manipulate light intensity, polarization, and phase in confined nanoscale geometries. Any technology that relies on optimal charge transport, or optical control and readout, including quantum devices for logic, sensing, and storage, may benefit from chiral quantum properties. These properties can be theoretically and experimentally investigated from a quantum information perspective, which has not yet been fully developed. There are uncharted implications for the quantum sciences once chiral couplings can be engineered to control the storage, transduction, and manipulation of quantum information. This forward-looking Review provides a survey of the experimental and theoretical fundamentals of chiral-influenced quantum effects and presents a vision for their possible future roles in enabling room-temperature quantum technologies.

Coexistence of structural and magnetic phases in van der Waals magnet CrI3.

CrI3 has raised as an important system to the emergent field of two-dimensional van der Waals magnetic materials. However, it is still unclear why CrI3 which has a ferromagnetic rhombohedral structure in bulk, changed to anti-ferromagnetic monoclinic at thin layers. Here we show that this behaviour is due to the coexistence of both monoclinic and rhombohedral crystal phases followed by three magnetic transitions at TC1 = 61 K, TC2 = 50 K and TC3 = 25 K. Each transition corresponds to a certain fraction of the magnetically ordered volume as well as monoclinic and rhombohedral proportion. The different phases are continuously accessed as a function of the temperature over a broad range of magnitudes. Our findings suggest that the challenge of understanding the magnetic properties of thin layers CrI3 is in general a coexisting structural-phase problem mediated by the volume-wise competition between magnetic phases already present in bulk.

Layer-Dependent Mechanical Properties and Enhanced Plasticity in the Van der Waals Chromium Trihalide Magnets.

The mechanical properties of magnetic materials are instrumental for the development of magnetoelastic theories and the optimization of strain-modulated magnetic devices. In particular, two-dimensional (2D) magnets hold promise to enlarge these concepts into the realm of low-dimensional physics and ultrathin devices. However, no experimental study on the intrinsic mechanical properties of the archetypal 2D magnet family of the chromium trihalides has thus far been performed. Here, we report the room temperature layer-dependent mechanical properties of atomically thin CrCl3 and CrI3, finding that the bilayers have Young's moduli of 62.1 and 43.4 GPa, highest sustained strains of 6.49% and 6.09% and breaking strengths of 3.6 and 2.2 GPa, respectively. This portrays the outstanding plasticity of these materials that is qualitatively demonstrated in the bulk crystals. The current study will contribute to the applications of the 2D magnets in magnetostrictive and flexible devices.

Mechanical Properties of Atomically Thin Tungsten Dichalcogenides: WS2, WSe2, and WTe2.

Two-dimensional (2D) tungsten disulfide (WS2), tungsten diselenide (WSe2), and tungsten ditelluride (WTe2) draw increasing attention due to their attractive properties deriving from the heavy tungsten and chalcogenide atoms, but their mechanical properties are still mostly unknown. Here, we determine the intrinsic and air-aged mechanical properties of mono-, bi-, and trilayer (1-3L) WS2, WSe2, and WTe2 using a complementary suite of experiments and theoretical calculations. High-quality 1L WS2 has the highest Young's modulus (302.4 ± 24.1 GPa) and strength (47.0 ± 8.6 GPa) of the entire family, overpassing those of 1L WSe2 (258.6 ± 38.3 and 38.0 ± 6.0 GPa, respectively) and WTe2 (149.1 ± 9.4 and 6.4 ± 3.3 GPa, respectively). However, the elasticity and strength of WS2 decrease most dramatically with increased thickness among the three materials. We interpret the phenomenon by the different tendencies for interlayer sliding in an equilibrium state and under in-plane strain and out-of-plane compression conditions in the indentation process, revealed by the finite element method and density functional theory calculations including van der Waals interactions. We also demonstrate that the mechanical properties of the high-quality 1-3L WS2 and WSe2 are largely stable in air for up to 20 weeks. Intriguingly, the 1-3L WSe2 shows increased modulus and strength values with aging in the air. This is ascribed to oxygen doping, which reinforces the structure. The present study will facilitate the design and use of 2D tungsten dichalcogenides in applications such as strain engineering and flexible field-effect transistors.

Properties and dynamics of meron topological spin textures in the two-dimensional magnet CrCl3.

Merons are nontrivial topological spin textures highly relevant for many phenomena in solid state physics. Despite their importance, direct observation of such vortex quasiparticles is scarce and has been limited to a few complex materials. Here, we show the emergence of merons and antimerons in recently discovered two-dimensional (2D) CrCl3 at zero magnetic field. We show their entire evolution from pair creation, their diffusion over metastable domain walls, and collision leading to large magnetic monodomains. Both quasiparticles are stabilized spontaneously during cooling at regions where in-plane magnetic frustration takes place. Their dynamics is determined by the interplay between the strong in-plane dipolar interactions and the weak out-of-plane magnetic anisotropy stabilising a vortex core within a radius of 8-10 nm. Our results push the boundary to what is currently known about non-trivial spin structures in 2D magnets and open exciting opportunities to control magnetic domains via topological quasiparticles.

Quantum Rescaling, Domain Metastability, and Hybrid Domain-Walls in 2D CrI3 Magnets.

Higher-order exchange interactions and quantum effects are widely known to play an important role in describing the properties of low-dimensional magnetic compounds. Here, the recently discovered 2D van der Waals (vdW) CrI3 is identified as a quantum non-Heisenberg material with properties far beyond an Ising magnet as initially assumed. It is found that biquadratic exchange interactions are essential to quantitatively describe the magnetism of CrI3 but quantum rescaling corrections are required to reproduce its thermal properties. The quantum nature of the heat bath represented by discrete electron-spin and phonon-spin scattering processes induces the formation of spin fluctuations in the low-temperature regime. These fluctuations induce the formation of metastable magnetic domains evolving into a single macroscopic magnetization or even a monodomain over surface areas of a few micrometers. Such domains display hybrid characteristics of Néel and Bloch types with a narrow domain wall width in the range of 3-5 nm. Similar behavior is expected for the majority of 2D vdW magnets where higher-order exchange interactions are appreciable.

Outstanding Thermal Conductivity of Single Atomic Layer Isotope-Modified Boron Nitride.

Materials with high thermal conductivities (κ) are valuable to solve the challenge of waste heat dissipation in highly integrated and miniaturized modern devices. Herein, we report the first synthesis of atomically thin isotopically pure hexagonal boron nitride (BN) and its one of the highest κ among all semiconductors and electric insulators. Single atomic layer (1L) BN enriched with ^{11}B has a κ up to 1009 W/mK at room temperature. We find that the isotope engineering mainly suppresses the out-of-plane optical (ZO) phonon scatterings in BN, which subsequently reduces acoustic-optical scatterings between ZO and transverse acoustic (TA) and longitudinal acoustic phonons. On the other hand, reducing the thickness to a single atomic layer diminishes the interlayer interactions and hence umklapp scatterings of the out-of-plane acoustic (ZA) phonons, though this thickness-induced κ enhancement is not as dramatic as that in naturally occurring BN. With many of its unique properties, atomically thin monoisotopic BN is promising on heat management in van der Waals devices and future flexible electronics. The isotope engineering of atomically thin BN may also open up other appealing applications and opportunities in 2D materials yet to be explored.