Near-room-temperature antiferromagnetism in Janus Fe$X$F ($X$ = O, S) monolayers

Abstract

Inspired by the recently synthesized hexagonal layered phase of FeF$_2$, we studied the magnetic properties of the 1T-FeF$_2$ monolayer and its Janus Fe$X$F ($X$ = O, S) derivatives by first-principles calculations. Our results confirm that these materials are antiferromagnetic semiconductors, and that anion substitution effectively tunes their material properties: the band gap shifts from 3.37 eV (direct, FeF$_2$) to 2.35 eV (direct, FeOF) and 1.13 eV (indirect, FeSF); the magnetic moment of Fe ions increases; and the N\'{e}el temperature ($T_N$) rises dramatically to 248 K (FeSF) and 207 K (FeOF). Janus structures exhibit enhanced magnetic moment and direct AFM coupling. Under compression, $T_N$ is further optimized to 274 K ($-2$\% strain, FeSF) and 244 K ($-5$\% strain, FeOF). Both Janus materials retain their semiconducting nature and direction of easy magnetization axis under $\pm5$\% strain. This study validates the Janus structure as a viable approach to enhance 2D antiferromagnetism and highlights Fe-based oxyhalides as promising spintronic materials.