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Abstract Electron band topology is combined with intrinsic magnetic orders in MnBi 2 Te 4 , leading to novel quantum phases. Here we investigate collective spin excitations (i.e. magnons) and spin fluctuations in atomically thin MnBi 2 Te 4 flakes using Raman spectroscopy. In a two-septuple layer with non-trivial topology, magnon characteristics evolve as an external magnetic field tunes the ground state through three ordered phases: antiferromagnet, canted antiferromagnet, and ferromagnet. The Raman selection rules are determined by both the crystal symmetry and magnetic order while the magnon energy is determined by different interaction terms. Using non-interacting spin-wave theory, we extract the spin-wave gap at zero magnetic field, an anisotropy energy, and interlayer exchange in bilayers. We also find magnetic fluctuations increase with reduced thickness, which may contribute to a less robust magnetic order in single layers. 

The van der Waals magnets CrX₃(X = I, Br, and Cl) exhibit highly tunable magnetic properties and are promising candidates for developing novel two‐dimensional (2D) spintronic devices such as magnetic tunnel junctions and spin tunneling transistors. Previous studies of the antiferromagnetic CrCl₃have mainly focused on mechanically exfoliated samples. Controlled synthesis of high quality atomically thin flakes is critical for their technological implementation but has not been achieved to date. This work reports the growth of large CrCl₃flakes down to monolayer thickness via the physical vapor transport technique. Both isolated flakes with well‐defined facets and long stripe samples with the trilayer portion exceeding 60 µm have been obtained. High‐resolution transmission electron microscopy studies show that the CrCl₃flakes are single crystalline in the monoclinic structure, consistent with the Raman results. The room temperature stability of the CrCl₃flakes decreases with decreasing thickness. The tunneling magnetoresistance of graphite/CrCl₃/graphite tunnel junctions confirms that few‐layer CrCl₃possesses in‐plane magnetic anisotropy and Néel temperature of 17 K. This study paves the path for developing CrCl₃‐based scalable 2D spintronic applications.

 

A long‐standing pursuit in materials science is to identify suitable magnetic semiconductors for integrated information storage, processing, and transfer. Van der Waals magnets have brought forth new material candidates for this purpose. Recently, sharp exciton resonances in antiferromagnet NiPS₃have been reported to correlate with magnetic order, that is, the exciton photoluminescence intensity diminishes above the Néel temperature. Here, it is found that the polarization of maximal exciton emission rotates locally, revealing three possible spin chain directions. This discovery establishes a new understanding of the antiferromagnet order hidden in previous neutron scattering and optical experiments. Furthermore, defect‐bound states are suggested as an alternative exciton formation mechanism that has yet to be explored in NiPS₃. The supporting evidence includes chemical analysis, excitation power, and thickness dependent photoluminescence and first‐principles calculations. This mechanism for exciton formation is also consistent with the presence of strong phonon side bands. This study shows that anisotropic exciton photoluminescence can be used to read out local spin chain directions in antiferromagnets and realize multi‐functional devices via spin‐photon transduction.