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 exhibit different ME coupling behavior. During the switching of polarization, the reversal of skyrmions chirality, the transition of the magnetic ground state from FM to antiferromagnetic, and the changes in spin-polarized electron 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.

新型二维（2D）多铁性材料的发现因其在实现信息存储和逻辑器件方面的潜力而具有吸引力。尽管已经探索了许多方法来同时将铁磁 (FM) 和铁电 (FE) 阶引入 2D 材料中，但所得系统经常受到弱磁电 (ME) 耦合或有限的室温稳定性的困扰。在这里，我们提出了一种构建非中心对称 AM ₂ X ₄ 多铁性单层的超晶格策略，即将过渡金属离子 (A) 插入过渡金属二硫属化物的四方空位中双层（MX ₂ ）。从 960 种插层 AM ₂ X ₄ 化合物开始，我们的高通量计算已识别出 21 种具有鲁棒磁序、大 FE 极化、低转变势垒、高 FE/FM 转变温度的多铁性材料，以及强ME耦合。根据磁性起源，我们将它们分为十二种a型、七种b型和两种c型多铁性材料，它们表现出不同的ME耦合行为。在极化切换过程中，在a型、b型和c型二维多铁性材料中观察到斯格明子手性的反转、磁基态从FM到反铁磁的转变以及自旋极化电子分布的变化材料，分别。这些结果极大地扩展了二维铁质材料系列，并为设计和实现非易失性逻辑和存储器件铺平了道路。