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

The niobium oxide polymorph T-Nb2O5 has been extensively investigated in its bulk form especially for applications in fast-charging batteries and electrochemical (pseudo)capacitors. Its crystal structure, which has two-dimensional (2D) layers with very low steric hindrance, allows for fast Li-ion migration. However, since its discovery in 1941, the growth of single-crystalline thin films and its electronic applications have not yet been realized, probably due to its large orthorhombic unit cell along with the existence of many polymorphs. Here we demonstrate the epitaxial growth of single-crystalline T-Nb2O5 thin films, critically with the ionic transport channels oriented perpendicular to the film's surface. These vertical 2D channels enable fast Li-ion migration, which we show gives rise to a colossal insulator-metal transition, where the resistivity drops by 11 orders of magnitude due to the population of the initially empty Nb 4d(0) states by electrons. Moreover, we reveal multiple unexplored phase transitions with distinct crystal and electronic structures over a wide range of Li-ion concentrations by comprehensive in situ experiments and theoretical calculations, which allow for the reversible and repeatable manipulation of these phases and their distinct electronic properties. This work paves the way for the exploration of novel thin films with ionic channels and their potential applications. The two-dimensional layered crystal structure of niobium oxide polymorph T-Nb2O5 exhibits fast Li-ion diffusion that is promising for energy storage applications. Epitaxial growth of single-crystalline T-Nb2O5 thin films with ionic transport channels oriented perpendicular to the surface are now demonstrated.

Automated summary

This study successfully demonstrates the epitaxial growth of single-crystalline T-Nb2O5 thin films with vertical 2D channels for fast Li-ion migration. The films exhibit a colossal insulator-metal transition due to the population of previously empty Nb 4d(0) states. In addition, multiple unexplored phase transitions with distinct crystal and electronic structures have been discovered, allowing for reversible and repeatable manipulation of these phases and their unique electronic properties.