Control over a Wide Phase Diagram of 2D Correlated Electrons by Surface Doping; K/1T-TaS₂

We demonstrate the systematic tuning of a trivial insulator into a Mott insulator and a Mott insulator into a correlated metallic and a pseudogap state, which emerge in a quasi-two-dimensional electronic system of 1T-TaS₂ through strong electron correlation. The band structure evolution is investigated upon surface doping by alkali adsorbates for two distinct phases occurring at around 220 and 10 K by angle-resolved photoelectron spectroscopy. We find contrasting behaviors upon doping that corroborate the fundamental difference of two electronic states: while the antibonding state of the spin-singlet insulator at 10 K is partially occupied to produce an emerging Mott insulating state, the presumed Mott insulating state at 220 K evolves into a correlated metallic state and then a pseudogap state. The work indicates that surface doping onto correlated 2D materials can be a powerful tool to systematically engineer a wide range of correlated electronic phases.