Probing Short-Range Correlations in the van der Waals Magnet CrSBr by Small-Angle Neutron Scattering

The layered metamagnet CrSBr offers a rich interplay between magnetic, optical, and electrical properties that can be extended down to the two-dimensional (2D) limit. Despite the extensive research regarding the long-range magnetic order in magnetic van der Waals materials, short-range correlations have been loosely investigated. By using small-angle neutron scattering (SANS) the formation of short-range magnetic regions in CrSBr with correlation lengths that increase upon cooling up to ≈3 nm at the antiferromagnetic ordering temperature (T _N  ≈ 140 K) is shown. Interestingly, these ferromagnetic correlations start developing below 200 K, i.e., well above T _N. Below T _N, these correlations rapidly decrease and are negligible at low-temperatures. The experimental results are well-reproduced by an effective spin Hamiltonian, which pinpoints that the short-range correlations in CrSBr are intrinsic to the monolayer limit, and discard the appearance of any frustrated phase in CrSBr at low-temperatures within the experimental window between 2 and 200 nm. Overall, the obtained results are compatible with a spin freezing scenario of the magnetic fluctuations in CrSBr and highlight SANS as a powerful technique for characterizing the rich physical phenomenology beyond the long-range order paradigm offered by van der Waals magnets.