Intrinsically Moiré-Patterned Two-Dimensional Polymorphic Networks for Modulated Charge Order and Proximity Superconductivity

Abstract Moiré superlattices provide a versatile route to engineering correlated electronic and topological states in van der Waals heterostructures, yet their use to organize structural polymorphism and phase-selective charge, magnetic, and superconducting states within a single two-dimensional material remains elusive. Here, we report modulated charge order and proximity superconductivity in an intrinsically moiré-patterned 1T/1T′ polymorphic network of monolayer VTe2 grown epitaxially on superconducting NbSe2. Scanning tunneling microscopy/spectroscopy and first-principles calculations show that in situ annealing of twist-moiré VTe2/NbSe2 creates alternating 1T and 1T′ domains. The origin of the selective 1T-to-1T′ conversion is due to the moiré-induced anisotropic strain. This moiré-registered network hosts phase-specific short-range charge orders: 4 × 4 in 1T and 3 × 3 in 1T′. In the proximity-superconducting regime, spatially modulated in-gap bound states and suppressed coherence peaks reveal phase-dependent magnetic pair breaking. This work establishes intrinsically moiré-patterned polymorphism as a route to programmable two-dimensional quantum materials.