Abstract
We report a tetragonal polymorph of synthesized under high pressures. This phase is structurally characterized by two-dimensional square nets that are sandwiched by sulfur atomic layers. The electrical, magnetic, and thermodynamic measurements indicate that it is an antiferromagnetic insulator with a Néel temperature of 121 K. A successive magnetic transition at is observed, possibly associated with spin canting due to Dzyaloshinskii-Moriya interactions. Density functional theory based calculations reveal Mott localization driven by the on-site electron-electron Coulomb repulsion. The calculations also suggest a noncollinear -spin structure with two- [ and ] propagation vectors, primarily due to the magnetocrystalline anisotropy as well as the next-nearest-neighbor superexchange interactions mediated by oxygen and sulfur anions, respectively.
2 More- Received 10 February 2022
- Revised 10 April 2022
- Accepted 3 May 2022
DOI:https://doi.org/10.1103/PhysRevMaterials.6.055002
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