Tailoring spontaneous symmetry breaking in engineered van der Waals superlattices

Abstract

Superlattice engineering in van der Waals heterostructures (e.\,g.\ by moiré engineering) provides a powerful platform for designing electronic bands and realising correlated and topological quantum phenomena. Here, we pioneer a scheme to tailor superpotentials based on intrinsic substrate electronic orders. We show that this establishes a robust, self-aligned, and highly versatile route to band-structure control as we demonstrate in graphene by engineering two distinct, nearly commensurate superlattices using the charge density waves of 1T-NbSe$_2$. In these superlattices the graphene's Dirac cones are folded either to the $Γ$-point or to the K-points of the mini-Brillouin zone. Using scanning tunnelling microscopy, we observe that the $Γ$-folded system preserves C$_3$ symmetry, while the K-folded system exhibits spontaneous symmetry breaking. Combining density functional theory with an interlayer interaction model, we reveal that this difference is not electronically driven but originates from a structural instability. Our work establishes superlattice engineering for designer quantum states and unveils a structural mechanism for controlled emergent symmetry breaking.