Gate tuning of coupled electronic and structural phase transition in atomically thin Ta2NiSe5

Realizing an excitonic insulator phase from narrow-gap semiconductors remains challenging, as unambiguous experimental signatures are difficult to establish. Ta2NiSe5 has been widely regarded as a leading candidate, yet the nature of its phase transition and insulating state remains controversial. Here, we report a systematic Raman spectroscopy study of Ta2NiSe5 as a function of thickness and field-effect doping, complemented by electrical transport measurements. The phase transition persists down to the monolayer limit, with the critical temperature increasing as thickness decreases. In bilayer samples, both electron and hole doping suppress the insulating state, with electron doping lowering and hole doping raising the transition temperature. Importantly, the quasi-elastic scattering, previously attributed to excitonic fluctuations, evolves monotonically across the entire doping range, inconsistent with the expected suppression of excitonic correlations by Coulomb screening. These findings rule out a dominant excitonic mechanism and instead point to a coupled electronic and structural phase transition, whose stability is tunable by carrier doping. Our doping-based approach offers a general strategy for evaluating the role of excitonic effects in candidate excitonic insulators. Ta2NiSe5 is an excitonic insulator candidate. Here, the authors rule out a dominant excitonic mechanism for this material and instead point to a coupled electronic and structural phase transition using a doping-based approach.