Designer three-dimensional electronic bands in asymmetric transition metal dichalcogenide heterostructures

Van der Waals materials enable the construction of atomically sharp interfaces between compounds with distinct crystal and electronic properties. This is dramatically exploited in moiré systems, where a lattice mismatch or twist between monolayers generates an emergent in-plane periodicity, giving rise to electronic properties absent in the constituent materials. In contrast, vertical superlattices, formed by stacking dissimilar materials in the out-of-plane direction on the nanometer scale, have received far less attention despite their potential to realize analogous emergent phenomena in three dimensions. Through angle-resolved photoemission spectroscopy and density functional theory, we investigate six-to-eight-layer transition metal dichalcogenide (TMD) heterostructures constructed from pairs of stacked few-layer materials. Counterintuitively, we find that even these single superlattice units can host fully-delocalised bands, evidencing a robust coherent interlayer coupling across lattice-mismatched interfaces over extended spatial scales. We show how uncompensated semimetallic phases and energetically-mismatched topological surface states are readily and exclusively stabilized within such asymmetrical architectures. These findings establish two-component heterostructures in the intermediate layer-regime as platforms to invoke and control unprecedented combinations and instances of the diverse quantum phases native to many-layer TMDs.