Multiferroicity in the two-dimensional limit in hexagonal LuFeO3 films

Abstract: Multiferroic oxides, which combine coupled ferroelectric and magnetic orders, are central to understanding correlated quantum phenomena. Yet, as thickness approaches the two-dimensional (2D) limit, both ferroelectricity and magnetism are conventionally expected to vanish due to depolarization fields and finite-size effects, respectively. Here, we demonstrate that hexagonal LuFeO3 (h-LuFeO3) retains coupled ferroelectricity and magnetism at the 2D limit, with a thickness of just one and a half unit cells. Remarkably, the ferroelectric polarization remains comparable to bulk values at room temperature, while long-range magnetism and magnetoelectric coupling persist at low temperatures. We further show that the K3 phonon mode, which mediates the polarization-magnetism coupling, is stable down to the 2D limit. Our results establish h-LuFeO3 as the first oxide system to exhibit genuine 2D-limit multiferroicity, providing a fundamental breakthrough in the long-standing quest to understand and control coupled ferroic orders at the atomic scale.