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.

The recent discovery of two-dimensional (2D) magnets [1][2][3] offers unique opportunities for the experimental exploration of low-dimensional magnetism 4 and the magnetic proximity effects 5,6 , and for the development of novel magnetoelectric, magnetooptic and spintronic devices 7,8 . These advancements call for 2D materials with diverse magnetic structures as well as effective probes for their magnetic symmetries, which is key to understanding intralayer magnetic order and interlayer magnetic coupling [9][10][11] . However, traditional techniques do not probe magnetic symmetry; these examples include magneto-optical Kerr effect 2,3 , reflective magnetic circular dichroism and Raman spectroscopy [12][13][14] , anomalous Hall effect 15 , tunneling magnetoresistance 16,17 , spin-polarized scanning tunneling microscopy 9 , and single-spin scanning magnetometry 18 . Here we apply second harmonic generation (SHG), a technique acutely sensitive to symmetry breaking, to probe the magnetic structure of a new 2D magnetic semiconductor, CrSBr. We find that CrSBr monolayers are ferromagnetically ordered below 146 K, an observation enabled by the discovery of a giant magnetic dipole SHG effect in the centrosymmetric 2D structure. In multilayers, the ferromagnetic monolayers are coupled antiferromagnetically, with the Néel temperature notably increasing with decreasing layer number. The magnetic structure of CrSBr, comprising spins co-aligned in-plane with rectangular unit cell, differs markedly from the prototypical 2D hexagonal magnets CrI3 and Cr2Ge2Te6 with out-of-plane moments.

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

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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.

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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 μ 0 H E = 0.395(2) T, and the hard and intermediate-axis anisotropy parameters are μ 0 H c = 1.30(2) T and μ 0 H a = 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.