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

Han, Hyeon; Jacquet, Quentin; Jiang, Zhen; Sayed, Farheen N.; Jeon, Jae-Chun; Sharma, Arpit; Schankler, Aaron M.; Kakekhani, Arvin; Meyerheim, Holger L.; Park, Jucheol; Nam, Sang Yeol; Griffith, Kent J.; Simonelli, Laura; Rappe, Andrew M.; Grey, Clare P.; Parkin, Stuart S.  P.

doi:10.1038/s41563-023-01612-2

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

Journal Article · 27 July 2023 · Nature Materials

DOI:https://doi.org/10.1038/s41563-023-01612-2· OSTI ID:2421101

^[1]; Jacquet, Quentin; ; Sayed, Farheen N.; Jeon, Jae-Chun; Sharma, Arpit; ; ; ; Park, Jucheol; Nam, Sang Yeol; ; ; ; ;

OSTI

Abstract

The niobium oxide polymorphT-Nb₂O₅has 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-crystallineT-Nb₂O₅thin 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 4d⁰states 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.

Research Organization:: Univ. of Pennsylvania, Philadelphia, PA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: SC0019281; AC02-06CH11357

OSTI ID:: 2421101

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 9 Vol. 22; ISSN 1476-1122

Publisher:: Springer Nature

Country of Publication:: United States

Language:: English

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

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

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