Perspective on computational design of two-dimensional materials with robust multiferroic coupling

Two-dimensional (2D) multiferroic materials with robust magnetoelectric coupling and controllable topological solitons (such as skyrmions) are promising candidates for advanced information storage and processing. Due to the limitations of experimental techniques, first-principles investigations stand out in answering fundamental questions of 2D multiferroic couplings, thus providing guidance for experimental validation. Herein, we will give a review of recent theoretical progress in the exploration of 2D multiferroic coupling via structural design and molecular engineering approach. Particularly, we will focus on (i) how to design the multiferroic structure in the 2D form; (ii) how to achieve robust magnetoelectric coupling; and (iii) how to electrically control the magnetic skyrmion via multiferroic effects. Finally, we give some perspectives on the remaining challenges and opportunities for predicting 2D multiferroic materials.