Coupling between magnetic order and charge transport in a two-dimensional magnetic semiconductor.

Semiconductors, featuring tunable electrical transport, and magnets, featuring tunable spin configurations, form the basis of many information technologies. A long-standing challenge has been to realize materials that integrate and connect these two distinct properties. Two-dimensional (2D) materials offer a platform to realize this concept, but known 2D magnetic semiconductors are electrically insulating in their magnetic phase. Here we demonstrate tunable electron transport within the magnetic phase of the 2D semiconductor CrSBr and reveal strong coupling between its magnetic order and charge transport. This provides an opportunity to characterize the layer-dependent magnetic order of CrSBr down to the monolayer via magnetotransport. Exploiting the sensitivity of magnetoresistance to magnetic order, we uncover a second regime characterized by coupling between charge carriers and magnetic defects. The magnetoresistance within this regime can be dynamically and reversibly tuned by varying the carrier concentration using an electrostatic gate, providing a mechanism for controlling charge transport in 2D magnets.

Anisotropic Gigahertz Antiferromagnetic Resonances of the Easy-Axis van der Waals Antiferromagnet CrSBr.

We report measurements of antiferromagnetic resonances in the van der Waals easy-axis antiferromagnet CrSBr. The interlayer exchange field and magnetocrystalline anisotropy fields are comparable to laboratory magnetic fields, allowing a rich variety of gigahertz-frequency dynamical modes to be accessed. By mapping the resonance frequencies as a function of the magnitude and angle of applied magnetic field, we identify the different regimes of antiferromagnetic dynamics. The spectra show good agreement with a Landau-Lifshitz model for two antiferromagnetically coupled sublattices, accounting for interlayer exchange and triaxial magnetic anisotropy. Fits allow us to quantify the parameters governing the magnetic dynamics: At 5 K, the interlayer exchange field is µ0HE = 0.395(2) T, and the hard and intermediate-axis anisotropy parameters are µ0Hc = 1.30(2) T and µ0Ha = 0.383(7) T. The existence of within-plane anisotropy makes it possible to control the degree of hybridization between the antiferromagnetic resonances using an in-plane magnetic field.

Interlayer electronic coupling on demand in a 2D magnetic semiconductor.

When monolayers of two-dimensional (2D) materials are stacked into van der Waals structures, interlayer electronic coupling can introduce entirely new properties, as exemplified by recent discoveries of moiré bands that host highly correlated electronic states and quantum dot-like interlayer exciton lattices. Here we show the magnetic control of interlayer electronic coupling, as manifested in tunable excitonic transitions, in an A-type antiferromagnetic 2D semiconductor CrSBr. Excitonic transitions in bilayers and above can be drastically changed when the magnetic order is switched from the layered antiferromagnetic ground state to a field-induced ferromagnetic state, an effect attributed to the spin-allowed interlayer hybridization of electron and hole orbitals in the latter, as revealed by Green's function-Bethe-Salpeter equation (GW-BSE) calculations. Our work uncovers a magnetic approach to engineer electronic and excitonic effects in layered magnetic semiconductors.

Magnetic Order and Symmetry in the 2D Semiconductor CrSBr.

The advent of two-dimensional (2D) magnets offers unprecedented control over electrons and spins. A key factor in determining exchange coupling and magnetic order is symmetry. Here, we apply second harmonic generation (SHG) to probe a 2D magnetic semiconductor CrSBr. We find that monolayers are ferromagnetically ordered below 146 K, an observation enabled by the discovery of a large magnetic dipole SHG effect in the centrosymmetric structure. In multilayers, the ferromagnetic monolayers are coupled antiferromagnetically, and in contrast to other 2D magnets, the Néel temperature of CrSBr increases with decreasing layer number. We identify magnetic dipole and magnetic toroidal moments as order parameters of the ferromagnetic monolayer and antiferromagnetic bilayer, respectively. These findings establish CrSBr as an exciting 2D magnetic semiconductor and extend the SHG probe of magnetic symmetry to the monolayer limit, opening the door to exploring the applications of magnetic-electronic coupling and the magnetic toroidal moment.

Polytypism, Anisotropic Transport, and Weyl Nodes in the van der Waals Metal TaFeTe4.

Layered van der Waals (vdW) materials belonging to the MM'Te4 structure class have recently received intense attention due to their ability to host exotic electronic transport phenomena, such as in-plane transport anisotropy, Weyl nodes, and superconductivity. Here we report two new vdW materials with strongly anisotropic in-plane structures featuring stripes of metallic TaTe2 and semiconducting FeTe2, α-TaFeTe4 and ß-TaFeTe4. We find that the structure of α-TaFeTe4 produces strongly anisotropic in-plane electronic transport (anisotropy ratio of up to 250%), outcompeting all other vdW metals, and demonstrate that it can be mechanically exfoliated to the two-dimensional (2D) limit. We also explore the possibility that broken inversion symmetry in ß-TaFeTe4 produces Weyl points in the electronic band structure. Eight Weyl nodes slightly below the Fermi energy are computationally identified for ß-TaFeTe4, indicating they may contribute to the transport behavior of this polytype. These findings identify the TaFeTe4 polytypes as an ideal platform for investigation of 2D transport anisotropy and chiral charge transport as a result of broken symmetry.

Exchange Bias Between van der Waals Materials: Tilted Magnetic States and Field-Free Spin-Orbit-Torque Switching.

Magnetic van der Waals heterostructures provide a unique platform to study magnetism and spintronics device concepts in the 2D limit. Here, studies of exchange bias from the van der Waals antiferromagnet CrSBr acting on the van der Waals ferromagnet Fe3GeTe2 (FGT) are reported. The orientation of the exchange bias is along the in-plane easy axis of CrSBr, perpendicular to the out-of-plane anisotropy of the FGT, inducing a strongly tilted magnetic configuration in the FGT. Furthermore, the in-plane exchange bias provides sufficient symmetry breaking to allow deterministic spin-orbit torque switching of the FGT in CrSBr/FGT/Pt samples at zero applied magnetic field. A minimum thickness of the CrSBr of >10 nm is needed to provide a non-zero exchange bias at 30 K.

Reversible strain-induced magnetic phase transition in a van der Waals magnet.

Mechanical deformation of a crystal can have a profound effect on its physical properties. Notably, even small modifications of bond geometry can completely change the size and sign of magnetic exchange interactions and thus the magnetic ground state. Here we report the strain tuning of the magnetic properties of the A-type layered antiferromagnetic semiconductor CrSBr achieved by designing a strain device that can apply continuous, in situ uniaxial tensile strain to two-dimensional materials, reaching several percent at cryogenic temperatures. Using this apparatus, we realize a reversible strain-induced antiferromagnetic-to-ferromagnetic phase transition at zero magnetic field and strain control of the out-of-plane spin-canting process. First-principles calculations reveal that the tuning of the in-plane lattice constant strongly modifies the interlayer magnetic exchange interaction, which changes sign at the critical strain. Our work creates new opportunities for harnessing the strain control of magnetism and other electronic states in low-dimensional materials and heterostructures.

Visualizing Atomically Layered Magnetism in CrSBr.

2D materials can host long-range magnetic order in the presence of underlying magnetic anisotropy. The ability to realize the full potential of 2D magnets necessitates systematic investigation of the role of individual atomic layers and nanoscale inhomogeneity (i.e., strain) on the emergence of stable magnetic phases. Here, spatially dependent magnetism in few-layer CrSBr is revealed using magnetic force microscopy (MFM) and Monte Carlo-based simulations. Nanoscale visualization of the magnetic sheet susceptibility is extracted from MFM data and force-distance curves, revealing a characteristic onset of both intra- and interlayer magnetic correlations as a function of temperature and layer-thickness. These results demonstrate that the presence of a single uncompensated layer in odd-layer terraces significantly reduces the stability of the low-temperature antiferromagnetic (AFM) phase and gives rise to multiple coexisting magnetic ground states at temperatures close to the bulk Néel temperature (TN ). Furthermore, the AFM phase can be reliably suppressed using modest fields (≈16 mT) from the MFM probe, behaving as a nanoscale magnetic switch. This prototypical study of few-layer CrSBr demonstrates the critical role of layer parity on field-tunable 2D magnetism and validates MFM for use in nanomagnetometry of 2D materials (despite the ubiquitous absence of bulk zero-field magnetism in magnetized sheets).

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.

Electrical and thermal generation of spin currents by magnetic bilayer graphene.

Ultracompact spintronic devices greatly benefit from the implementation of two-dimensional materials that provide large spin polarization of charge current together with long-distance transfer of spin information. Here spin-transport measurements in bilayer graphene evidence a strong spin-charge coupling due to a large induced exchange interaction by the proximity of an interlayer antiferromagnet (CrSBr). This results in the direct detection of the spin polarization of conductivity (up to 14%) and a spin-dependent Seebeck effect in the magnetic graphene. The efficient electrical and thermal spin-current generation is the most technologically relevant aspect of magnetism in graphene, controlled here by the antiferromagnetic dynamics of CrSBr. The high sensitivity of spin transport in graphene to the magnetization of the outermost layer of the adjacent antiferromagnet, furthermore, enables the read-out of a single magnetic sublattice. The combination of gate-tunable spin-dependent conductivity and Seebeck coefficient with long-distance spin transport in a single two-dimensional material promises ultrathin magnetic memory and sensory devices based on magnetic graphene.

Layered Antiferromagnetism Induces Large Negative Magnetoresistance in the van der Waals Semiconductor CrSBr.

The recent discovery of magnetism within the family of exfoliatable van der Waals (vdW) compounds has attracted considerable interest in these materials for both fundamental research and technological applications. However, current vdW magnets are limited by their extreme sensitivity to air, low ordering temperatures, and poor charge transport properties. Here the magnetic and electronic properties of CrSBr are reported, an air-stable vdW antiferromagnetic semiconductor that readily cleaves perpendicular to the stacking axis. Below its Néel temperature, TN  = 132 ± 1 K, CrSBr adopts an A-type antiferromagnetic structure with each individual layer ferromagnetically ordered internally and the layers coupled antiferromagnetically along the stacking direction. Scanning tunneling spectroscopy and photoluminescence (PL) reveal that the electronic gap is ΔE  = 1.5 ± 0.2 eV with a corresponding PL peak centered at 1.25 ± 0.07 eV. Using magnetotransport measurements, strong coupling between magnetic order and transport properties in CrSBr is demonstrated, leading to a large negative magnetoresistance response that is unique among vdW materials. These findings establish CrSBr as a promising material platform for increasing the applicability of vdW magnets to the field of spin-based electronics.