Multiferroic Metallic Monolayer Cu(CrSe2)2

The two-dimensional (2D) Cu(CrSe$_2$)$_2$ monolayer stands out for its combined ferromagnetic (FM), ferroelectric (FE), and metallic properties, marking itself as a prominent 2D multiferroic metal. This work studies those properties and the relevant physics, using density functional calculations, Monte Carlo simulations, and $ab$ $initio$ molecular dynamics. Our results show that Cu(CrSe$_2$)$_2$ monolayer is in the Cr$^{3+}$ $t_{2g}^3$ state with $S$ = 3/2 and Cu$^{1+}$ $3d^{10}$ with $S$ = 0. A ligand hole in the Se 4$p$ orbitals gives rise to metallic behavior and enhances the FM coupling between the local Cr$^{3+}$ $S$ = 3/2 spins. The observed in-plane magnetic anisotropy primarily arises from exchange anisotropy, which is associated with the Cr-Se-Cr itinerant ferromagnetism. In contrast, both single-ion anisotropy and shape magnetic anisotropy contribute negligibly. The Dzyaloshinskii-Moriya interaction is also quite weak, only about 3\% of the intralayer exchange parameters. Our Monte Carlo simulations show a FM Curie temperature ($T_{\rm C}$) of 190 K. Moreover, the monolayer exhibits a vertical FE polarization of 1.79 pC/m and a FE polarization switching barrier of 182 meV/f.u., and the FE state remains stable above 800 K as shown by $ab$ $initio$ molecular dynamics simulations. Furthermore, a magnetoelectric coupling is partially manifested by a magnetization rotation from in-plane to out-of-plane associated with a FE-to-paraelectric transition. The magnetization rotation can also be induced by either hole or electron doping, and the hole doping increases the $T_{\rm C}$ up to 238 K. In addition, tensile strain reduces the FE polarization but enhances $T_{\rm C}$ to 290 K, while a compressive strain gives an opposite effect. Therefore, the multiferroic metallic Cu(CrSe$_2$)$_2$ monolayer may be explored for advanced multifunctional electronic devices.
Comment: 14 pages, 7 figures