Nonvolatile switching of intra- and interlayer magnetism in 2D CrSe2/Sc2CO2 multiferroic heterostructures

Abstract

Two-dimensional (2D) multiferroic van der Waals (vdW) heterostructures offer a highly promising platform for next-generation low-power nanoelectronics and spintronic devices. However, achieving robust magnetoelectric coupling in these systems remains a significant challenge due to the weak interlayer vdW interactions. In this work, using first-principles calculations, we report the nonvolatile electrical switching of both intralayer and interlayer magnetism in a multiferroic heterostructure composed of 2D ferroelectric Sc₂CO₂ and monolayer (1L-)/bilayer (2L-) CrSe₂. Specifically, in the 1L-CrSe₂/Sc₂CO₂ heterostructure, the polarization switch from P_↑ to P_↓ drives a transition from zigzag antiferromagnetic (zAFM) to ferromagnetic (FM) order and rotates the easy axis from in-plane to out-of-plane, while in the 2L-CrSe₂/Sc₂CO₂ heterostructure, it induces an interlayer transition from AFM to FM coupling. In-depth mechanistic analysis reveals that these magnetic phase transitions primarily stem from the polarization-induced structural modification, including changes in in-plane lattice constants and interlayer spacing, rather than conventional charge transfer. Our work establishes a feasible strategy, governed by structural modulation, for designing 2D multiferroic vdW heterostructures with robust magnetoelectric coupling.