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The niobium oxide polymorph T-Nb2O5 has been extensively investigated in itsbulk form especially for applications in fast-charging batteries andelectrochemical (pseudo)capacitors. Its crystal structure that hastwo-dimensional (2D) layers with very low steric hindrance allows for fastLi-ion migration. However, since its discovery in 1941, the growth ofsingle-crystalline thin films and its electronic applications have not yet beenrealized, likely due to its large orthorhombic unit cell along with theexistence of many polymorphs. Here we demonstrate the epitaxial growth ofsingle-crystalline T-Nb2O5 thin films, critically with the ionic transportchannels oriented perpendicular to the film's surface. These vertical 2Dchannels enable fast Li-ion migration which we show gives rise to a colossalinsulator-metal transition where the resistivity drops by eleven orders ofmagnitude due to the population of the initially empty Nb 4d0 states byelectrons. Moreover, we reveal multiple unexplored phase transitions withdistinct crystal and electronic structures over a wide range of Li-ionconcentrations by comprehensive in situ experiments and theoreticalcalculations, that allow for the reversible and repeatable manipulation ofthese phases and their distinct electronic properties. This work paves the wayto the exploration of novel thin films with ionic channels and their potentialapplications.

Li iontronics in single-crystalline T-Nb2O5 thin films with vertical ionic transport channels