Tuning competing electronic phases in monolayer VSe$_2$ via interface hybridization

Abstract

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 VSe$_2$ 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 moir\'e modulations. In contrast, bilayers preserve the in-plane $4a \times 4a$ CDW characteristic of the bulk limit. Strained, electronically decoupled monolayers formed in suspended membrane and bubble regions stabilize a $\sqrt{3}a\times\sqrt{7}a$ CDW phase, underscoring the reversible role of substrate interaction and hybridization.