Nonvolatile Electric Control of Ferromagnetism in Van Der Waals Multiferroic Heterostructures at Room Temperature

Abstract Multiferroic heterostructures offer a promising platform for next‐generation low‐power spintronic devices by enabling electric‐field control of magnetism. While recent advances in two‐dimensional (2D) van der Waals (vdW) magnetic and ferroelectric materials have sparked significant interest, achieving reliable and nonvolatile electrical modulation of magnetism at room temperature within vdW multiferroic heterostructures remains a substantial challenge. Here, this study demonstrates robust, reproducible, and nonvolatile electrical control of ferromagnetism in Fe3GaTe2/CuInP2S6 multiferroic heterostructures under ambient conditions. The modulation is evidenced macroscopically by reshaped magnetic hysteresis loops in anomalous Hall voltage measurements and microscopically by in situ magnetic and electric field‐induced domain evolution captured via magnetic force microscopy. The first‐principles calculations reveal that the polarization of CuInP2S6 induces a significant modulation of the Dzyaloshinskii‐Moriya interaction (DMI) in Fe3GaTe2. Incorporating these effects into micromagnetic simulations reproduces key features of the experimental hysteresis behaviors, indicating that the polarization‐enhanced DMI lowers domain wall formation energy and drives a transition from coherent to incoherent magnetic reversal. These findings not only surmount the challenge of electrically modulating ferromagnetism in vdW systems via remanent ferroelectric polarization at room temperature but also open new pathways for energy‐efficient skyrmion manipulation and vdW spintronic device engineering.