Revealing 2D Magnetism in a Bulk CrSBr Single Crystal by Electron Spin Resonance

Abstract

2D magnets represent material systems in which magnetic order and topological phase transitions can be observed. Based on these phenomena, novel types of computing architectures and magnetoelectronic devices can be envisaged. Unlike conventional magnetic films, their magnetism is independent of the substrate and interface qualities, and 2D magnetic properties manifest even in formally bulk single crystals. However, 2D magnetism in layered materials is rarely reported often due to weak exchange interactions and magnetic anisotropy, and low magnetic transition temperatures. Here, the electron spin resonance (ESR) properties of a layered antiferromagnetic CrSBr single crystal are reported. The W‐like shape angular dependence of the ESR linewidth provides a signature for room temperature spin–spin correlations and for the XY spin model. By approaching the Néel temperature the arising of competing intralayer ferromagnetic and interlayer antiferromagnetic interactions might lead to the formation of vortex and antivortex pairs. This argument is inferred by modeling the temperature dependence of the ESR linewidth with the topological Berezinskii‐Kosterlitz‐Thouless phase transition. These findings together with the chemical stability and semiconducting properties, make CrSBr a promising layered magnet for future magneto‐ and topological‐electronics.

Two-Dimensional Room-Temperature Magnetism in Janus Mn2I3S3 and Cr2I3Se3 Monolayers with Tunable Magnetic Properties by Strain Engineering

“…Recently, the preparation of two-dimensional Janus materials, such as MoSSe and CrSBr has become common. This provides us with two potential synthesis routes: (1) MoSSe-type, based on atomic substitution of the host material.…”

Ferromagnetic Interlayer Coupling in CrSBr Crystals Irradiated by Ions

“…Three characteristic modes, attributed to the A g modes of the out-of-plane vibration, can be clearly identified in the Raman spectra (cf. Figure b,c,d) . The A g 1 (113.8 cm –1 ) and A g 3 (342.5 cm –1 ) modes show maximum intensity when the laser polarization is parallel to the b -axis, while the A g 2 (245.2 cm –1 ) mode is most pronounced when the polarization is aligned with the a -axis, reflecting the strong structural anisotropy of the crystal structure.…”

Single crystal synthesis and properties of the two-dimensional van der Waals frustrated magnets, Mn2In2Se5 and Mn2Ga2S5

“…[16][17][18][19] Multiple avenues have been explored to design materials that are more robust to ambient conditions including capping with air stable hBN layers and using air stable transition metal dichalcogenides as hosts for magnetic doping. [20][21][22][23][24][25] Additionally, recent work has led to the identification of 2D vdW compounds that are inherently more resilient towards oxidation including CrSBr [26][27][28] and the MPCh 3 (Ch = S, Se, Te) family. 29,30 Most of these systems are ordered magnetic systems with either ferromagnetic or antiferromagnetic long-range ordering and minimal degrees of magnetic frustration.…”