High-temperature ferromagnetism and ferroelasticity in ultraflexible atomically thin square-shaped lattices

Abstract: The coexistence of high-temperature intrinsic ferromagnetic ordering, large magnetic anisotropy, along with novel mechanical properties such as ferroelasticity and flexibility, in experimental feasible two-dimensional (2D) crystals is greatly appealing for nanoscale spintronics. However, the progress in identifying such materials is limited. Here, by first-principles calculations, we report the findings of an extraordinary combination of the above qualities for the first time in a new 2D exfoliated FeSi nanosheet in the P4/nmm space group. Due to the strong anion-mediated superexchange interaction, the monolayer FeSi (ML-FeSi) exhibits a Curie temperature Tc as high as 830 K, surpassing the current experimental record (344 K for ML-Cr3Te4). Furthermore, including FeSi, such isostructural lattices all demonstrate exceptional softness, as evidenced by their ultra-low in-plane stiffness. Remarkably, the transition metal atom and square-shaped crystal form work together to give this family of ML materials unique properties that can transition from Ising-like 2D ferromagnets in FeSi, MnP, MnAs, CrP, FeI, and VAs to 2D-XY ones in CrAs, VP, and multiferroic MnGe and TiTe. Overall, our work highlights such 2D lattices as promising candidates in emerging multifunctional device applications and nontrivial topological spintronics.