Evidence of ferroelectricity in an antiferromagnetic vanadium trichloride monolayer

A reduced dimensionality of multiferroic materials is highly desired for device miniaturization, but the coexistence of ferroelectricity and magnetism at the two-dimensional limit is yet to be conclusively demonstrated. Here, we used a NbSe₂ substrate to break both the <i>C</i>₃ rotational and inversion symmetries in monolayer VCl₃ and, thus, introduced exceptional in-plane ferroelectricity into a two-dimensional magnet. Scanning tunneling spectroscopy directly visualized ferroelectric domains and manipulated their domain boundaries in monolayer VCl₃, where coexisting antiferromagnetic order with canted magnetic moments was verified by vibrating sample magnetometer measurements. Our density functional theory calculations highlight the crucial role that highly directional interfacial Cl-Se interactions play in breaking the symmetries and, thus, in introducing in-plane ferroelectricity, which was further verified by examining an ML-VCl₃/graphene sample. Our work demonstrates an approach to manipulate the ferroelectric states in monolayered magnets through van der Waals interfacial interactions.