Realization of 2D Multiferroic with Strong Magnetoelectric Coupling by Intercalation: A First-principles High-throughput Prediction

Abstract

The discovery of novel two-dimensional (2D) multiferroic materials is attractive due to their potential for the realization of information storage and logic devices. Although many approaches have been explored to simultaneously introduce ferromagnetic (FM) and ferroelectric (FE) orders into a 2D material, the resulting systems are often plagued by weak magnetoelectric (ME) coupling or limited room-temperature stability. Here, we present a superlattice strategy to construct non-centrosymmetric AM₂X₄ multiferroic monolayers, i.e., intercalating transition metal ions (A) into the tetragonal-like vacancies of transition metal dichalcogenide bilayers (MX₂). Starting from 960 intercalated AM₂X₄ compounds, our high-throughput calculations have identified 21 multiferroics with robust magnetic order, large FE polarization, low transition barrier, high FE/ FM transition temperature, and strong ME coupling. According to the origin of magnetism, we have classified them into twelve type-a, seven type-b, and two type-c multiferroics, which also exhibit different ME coupling behavior. During the switching of polarization, the reversal of skyrmions chirality, the transition of magnetic ground state from FM to antiferromagnetic, and the changes in spin polarized electron spatial distribution were observed in type-a, type-b, and type-c 2D multiferroic materials, respectively. These results substantially expand the family of 2D ferroic materials and pave an avenue for designing and implementing nonvolatile logic and memory devices.