Moiré-driven multiferroic order in twisted CrCl3, CrBr3 and CrI3 bilayers

Layered van der Waals materials have risen as a powerful platform to engineer artificial competing states of matter. Here we show the emergence of multiferroic order in twisted chromium trihalide bilayers, an order fully driven by the moiré pattern and absent in aligned multilayers. Using a combination of spin models and ab initio calculations, we show that a spin texture is generated in the moiré supercell of the twisted system as a consequence of the competition between stacking-dependent interlayer magnetic exchange and magnetic anisotropy. An electric polarization arises associated with such a non-collinear magnetic state due to the spin–orbit coupling, leading to the emergence of a local ferroelectric order following the moiré. Among the stochiometric trihalides, our results show that twisted CrBr3 bilayers give rise to the strongest multiferroic order. We further show the emergence of a strong magnetoelectric coupling, which allows the electric generation and control of magnetic skyrmions. Our results put forward twisted chromium trihalide bilayers, and in particular CrBr3 bilayers, as a powerful platform to engineer artificial multiferroic materials and electrically tunable topological magnetic textures.