Distinct electronic structure of the electrolyte gate-induced conducting phase in vanadium dioxide revealed by high-energy photoelectron spectroscopy

The development of new phases of matter at oxide interfaces and surfaces by extrinsic electric fields is of considerable significance both scientifically and technologically. Vanadium dioxide (VO₂), a strongly correlated material, exhibits a temperature-driven metal-to-insulator transition, which is accompanied by a structural transformation from rutile (high-temperature metallic phase) to monoclinic (low-temperature insulator phase). Recently, it was discovered that a low-temperature conducting state emerges in VO₂ thin films upon gating with a liquid electrolyte. Using photoemission spectroscopy measurements of the core and valence band states of electrolyte-gated VO₂ thin films, we show that electronic features in the gate-induced conducting phase are distinct from those of the temperature-induced rutile metallic phase. Moreover, polarization-dependent measurements reveal that the V 3d orbital ordering, which is characteristic of the monoclinic insulating phase, is partially preserved in the gate-induced metallic phase, whereas the thermally induced metallic phase displays no such orbital ordering. Angle-dependent measurements show that the electronic structure of the gate-induced metallic phase persists to a depth of at least ∼40 Å, the escape depth of the high-energy photoexcited electrons used here. The distinct electronic structures of the gate-induced and thermally induced metallic phases in VO₂ thin films reflect the distinct mechanisms by which these states originate. The electronic characteristics of the gate-induced metallic state are consistent with the formation of oxygen vacancies from electrolyte gating.