Moiré‐Induced Symmetry Breaking of Charge Order in van der Waals Heterostructures

ABSTRACT Layered materials that stack different lattice symmetries are rare in nature. Misfit layered chalcogenides, which combine square and hexagonal lattices of rocksalt monochalcogenides and transition‐metal dichalcogenides, provide a platform to explore how incommensurability and explicit symmetry breaking impact collective electronic phases. Here we use low‐temperature scanning tunneling microscopy/spectroscopy to probe the misfit compounds (MS) 1+δ TaS 2 with M = Pb, Sn and track how the misfit interface reshapes the electronic ground state of the embedded 1H‐TaS 2 monolayers. High‐resolution STM imaging and Fourier analysis reveal that the charge‐density wave (CDW) is incommensurate and exhibits spatially inhomogeneous, short‐range correlations. Strikingly, the CDW exhibits a pronounced and anisotropic response to the uniaxial moiré potential imposed by the misfit layer: its coherence lengths and ordering wavevectors become inequivalent, demonstrating a strong nonlinear coupling between the intrinsic CDW instability and the symmetry‐breaking moiré field. First‐principles‐informed multiscale modeling suggests that this reorganization arises from the combined effect of interlayer charge transfer and the spatially anisotropic energy landscape introduced by the misfit interface. In contrast, superconductivity is comparatively insensitive to the moiré, revealing a uniform, single full‐gap consistent with s‐wave pairing. Our results establish heterosymmetry stacking as a route to engineer correlated states in van der Waals materials.