Realizing Intralayer Magnetoelectric Coupling in Two-Dimensional Frustrated Multiferroic Heterostructures

Recent studies have demonstrated the ability to switch weakly coupled interlayer magnetic orders by using electric polarization in insulating van der Waals heterostructures. However, controlling strongly coupled intralayer magnetic orders remains a significant challenge. In this work, we propose that frustrated multiferroic heterostructures can exhibit enhanced intralayer magnetoelectric coupling. Through first-principles calculations, we have investigated a heterostructure composed of MnBr₂ and Nb₃I₈, wherein there is a competition between frustrated intralayer magnetic orders within the MnBr₂ and interlayer magnetic coupling via a unique spin-local field effect. As a result, manipulating the vertical electric polarization of the Nb₃I₈ layer successfully controls the ground-state intralayer magnetic order in the frustrated MnBr₂ layer, inducing transitions between zigzag antiferromagnetic and ferromagnetic orders. Our findings offer a novel approach to controlling intralayer spin structures, paving the way for advancements in spintronic applications in a single atomic layer, which cannot be achieved by interlayer magnetoelectric coupling.