Magnetic and Multiferroic Properties of Two-Dimensional FePX3 and CuFeP2X6 (X = S, Se, and Te)

Two-dimensional (2D) multiferroic materials have significant application potential for novel storage devices due to their tunable magnetic and ferroelectric properties. Transition metal phosphorus chalcogenides MPX3 (X = S, Se, and Te) were found to be magnetic and multiferroic with excellent tunability, promising for multifunctionalized applications. In this study, we investigated the antiferromagnetic and antiferroelectric properties of two-dimensional FePX3 and CuFeP2X6 by density functional theory. Monolayer FePS3/FePSe3 and FePTe3 take intralayer zigzag and Neel antiferromagnetic ground states, respectively. This tunability of intralayer magnetism results from the competition between the spin-exchange interactions of the first and second nearest Fe atoms. Bilayer FePX3 shows weak interlayer interactions and keeps electronic and magnetic characteristics similar to those of the monolayer. Moreover, by introducing the nonmagnetic Cu atom into FePX3, the inversion symmetry broken induces CuFeP2X6 to be multiferroic materials. The transition barrier between ferroelectric (FE) and antiferroelectric (AFE) phases in CuFeP2S6 and CuFeP2Se6 is 0.09 and 0.04 eV/f.u., similar to well-known multiferroic CuCrP2S6. FE-to-AFE phase transition is expected to be achieved by applying an electric field and uniaxial strain. CuFeP2Te6 shows the ground state with a distorted paraelectric phase. Our results show the fundamental properties and in-depth understanding of 2D FePX3 and CuFeP2X6, guiding further investigation of 2D multifunctionalized magnetoelectric devices.