Interaction-driven electronic ferroelectricity in van der Waals heterostructures

Abstract

Strong electronic correlations in narrow-band systems provide a promising route to realize emergent quantum phases. While ferroelectricity in van der Waals materials is typically associated with inversion symmetry breaking driven by lattice distortions, interlayer sliding, or moiré reconstruction, the possibility of generating ferroelectricity directly from electronic interactions remains largely unexplored. Here, using molecular beam epitaxy, scanning tunneling microscopy, and ab initio calculations, we investigate two stacking geometries of bilayer 1T-TaSe$_2$, A-C and A-C$'$, formed by coupled Star-of-David charge density wave phases. We show that both stackings realize quasi-one-dimensional interacting chains, but are governed by distinct interaction mechanisms. In the A-C stacking, strong interlayer hybridization leads to dimerization and the formation of a band insulating state. In contrast, the A-C$'$ stacking is dominated by interlayer Coulomb interactions, producing a spontaneous charge imbalance between layers that gives rise to an out-of-plane ferroelectric polarization. Furthermore, we demonstrate that ferroelectric and antiferroelectric interchain configurations can be stabilized and electrically switched by an external field. Our results prove that bilayer 1T-TaSe$_2$ is a platform for interaction-driven electronic ferroelectricity, establishing an overlooked family of charge-ordered correlated states in 1T-TaSe$_2$ multilayers.