Multiferroic Metallic Monolayer Cu(CrSe2)2

TL;DR

This study investigates the multiferroic metallic properties of a 2D Cu(CrSe2)2 monolayer, revealing its magnetic, ferroelectric, and tunable characteristics through computational methods, with potential applications in electronic devices.

Contribution

It provides the first detailed theoretical analysis of the multiferroic metallic Cu(CrSe2)2 monolayer, highlighting its magnetic and ferroelectric properties and their tunability.

Findings

Curie temperature of 190 K for ferromagnetism

Vertical ferroelectric polarization of 1.79 pC/m

Tensile strain increases T_C to 290 K

Abstract

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. 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 room temperature 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.