Tuning Competing Electronic Phases in Monolayer VSe2 via Interface Hybridization.

Competing electronic phases in two-dimensional transition metal dichalcogenides constitute a fertile platform for uncovering emergent ground states and elucidating the control parameters that govern the correlated electron phases. Among these materials, vanadium diselenide is particularly compelling: while the bulk hosts a well-established charge density wave (CDW), monolayers exhibit markedly different electronic behavior. Here, we identify three distinct electronic regimes in mechanically exfoliated VSe2 flakes on Au(111) substrates, where interfacial hybridization, charge transfer, and strain act as primary tuning parameters of electronic order. Monolayers strongly coupled to gold show complete suppression of the CDW, accompanied by the emergence of moiré modulations. In contrast, bilayers preserve the in-plane 4a × 4a CDW characteristic of the bulk limit. Strained, electronically decoupled monolayers formed in suspended membrane and bubble regions stabilize a √3a × √7a CDW phase, underscoring the reversible role of substrate interaction and hybridization.