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The single-layer FeSe/SrTiO3 (FeSe/STO) films have attracted much attentionbecause of their simple crystal structure, distinct electronic structure andrecord high superconducting transition temperature (Tc). The origin of thedramatic Tc enhancement in single-layer FeSe/STO films and the dichotomy ofsuperconductivity between single-layer and multiple-layer FeSe/STO films arestill under debate. Here we report a comprehensive high resolutionangle-resolved photoemission spectroscopy and scanning tunnelingmicroscopy/spectroscopy measurements on the electronic structure evolution withdoping in single-layer and multiple-layer FeSe/STO films. We find that thesingle-layer FeSe/STO films have a distinct parent phase and a route of dopingevolution to superconductivity that are fundamentally different frommultiple-layer FeSe/STO films. The parent phase of the single-layer FeSe/STOfilms is insulating, and its doping evolution is very similar to that of dopinga Mott insulator in cuprate superconductors. In multiple-layer FeSe/STO films,high-Tc superconductivity occurs by suppressing the nematic order in the parentcompound with electron doping. The single-layer FeSe/STO films represent thefirst clear case in the iron-based superconductors that the parent compound isan insulator. Our observations of the unique parent state and doping evolutionin the single-layer FeSe/STO films provide key insight in understanding itsrecord high-Tc superconductivity. They also provide a new route of realizingsuperconductivity in iron-based superconductors that is common in hightemperature cuprate superconductors.

Insulating Parent Phase and Distinct Doping Evolution to Superconductivity in Single-Layer FeSe/SrTiO3 Films