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Compelling evidence suggests distinct correlated electron behavior may existonly in clean 2D materials such as 1T-TaS2. Unfortunately, experiment andtheory suggest that extrinsic disorder in free standing 2D layers disruptscorrelation-driven quantum behavior. Here we demonstrate a route to realizingfragile 2D quantum states through endotaxial polytype engineering of van derWaals materials. The true isolation of 2D charge density waves (CDWs) betweenmetallic layers stabilizes commensurate long-range order and lifts the couplingbetween neighboring CDW layers to restore mirror symmetries via interlayer CDWtwinning. The twinned-commensurate charge density wave (tC-CDW) reported hereinhas a single metal--insulator phase transition at ~350 K as measuredstructurally and electronically. Fast in-situ transmission electron microscopyand scanned nanobeam diffraction map the formation of tC-CDWs. This workintroduces endotaxial polytype engineering of van der Waals materials to accesslatent 2D ground states distinct from conventional 2D fabrication.

Two-dimensional charge order stabilized in clean polytype heterostructures