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Evolution of Insulator-Metal Phase Transitions in Epitaxial Tungsten Oxide Films during Electrolyte-Gating

An interface between an oxide and an electrolyte gives rise to various processes as exemplified by electrostatic charge accumulation/depletion and electrochemical reactions such as intercalation/decalation under electric field. Here we directly compare typical device operations of those in electric double layer transistor geometry by adopting ${A}$-site vacant perovskite WO$_3$ epitaxial thin films as a channel material and two different electrolytes as gating agent. $\textit{In situ}$ measurements of x-ray diffraction and channel resistance performed during the gating revealed that in both the cases WO$_3$ thin film reaches a new metallic state through multiple phase transitions, accompanied by the change in out-of-plane lattice constant. Electrons are electrostatically accumulated from the interface side with an ionic liquid, while alkaline metal ions are more uniformly intercalated into the film with a polymer electrolyte. We systematically demonstrate this difference in the electrostatic and electrochemical processes, by comparing doped carrier density, lattice deformation behavior, and time constant of the phase transitions.