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Mechanisms of Hysteresis and Reversibility across the Voltage-Driven Perovskite-Brownmillerite Transformation in Electrolyte-Gated Ultrathin La0.5Sr0.5CoO3-δ.
Postiglione, William M; Yu, Guichuan; Chaturvedi, Vipul; Zhou, Hua; Heltemes, Kei; Jacobson, Andrew; Greven, Martin; Leighton, Chris.
Afiliación
  • Postiglione WM; Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, Minnesota 55455, United States.
  • Yu G; Minnesota Supercomputing Institute, University of Minnesota, Minneapolis, Minnesota 55455, United States.
  • Chaturvedi V; Characterization Facility, University of Minnesota, Minneapolis, Minnesota 55455, United States.
  • Zhou H; Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, Minnesota 55455, United States.
  • Heltemes K; Advanced Photon Source, Argonne National Laboratory, Lemont, Illinois 60439, United States.
  • Jacobson A; Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, Minnesota 55455, United States.
  • Greven M; Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, Minnesota 55455, United States.
  • Leighton C; School of Physics and Astronomy, University of Minnesota, Minneapolis, Minnesota 55455, United States.
ACS Appl Mater Interfaces ; 16(15): 19184-19197, 2024 Apr 17.
Article en En | MEDLINE | ID: mdl-38564510
ABSTRACT
Perovskite cobaltites have emerged as archetypes for electrochemical control of materials properties in electrolyte-gate devices. Voltage-driven redox cycling can be performed between fully oxygenated perovskite and oxygen-vacancy-ordered brownmillerite phases, enabling exceptional modulation of the crystal structure, electronic transport, thermal transport, magnetism, and optical properties. The vast majority of studies, however, have focused heavily on the perovskite and brownmillerite end points. In contrast, here we focus on hysteresis and reversibility across the entire perovskite ↔ brownmillerite topotactic transformation, combining gate-voltage hysteresis loops, minor hysteresis loops, quantitative operando synchrotron X-ray diffraction, and temperature-dependent (magneto)transport, on ion-gel-gated ultrathin (10-unit-cell) epitaxial La0.5Sr0.5CoO3-δ films. Gate-voltage hysteresis loops combined with operando diffraction reveal a wealth of new mechanistic findings, including asymmetric redox kinetics due to differing oxygen diffusivities in the two phases, nonmonotonic transformation rates due to the first-order nature of the transformation, and limits on reversibility due to first-cycle structural degradation. Minor loops additionally enable the first rational design of an optimal gate-voltage cycle. Combining this knowledge, we demonstrate state-of-the-art nonvolatile cycling of electronic and magnetic properties, encompassing >105 transport ON/OFF ratios at room temperature, and reversible metal-insulator-metal and ferromagnet-nonferromagnet-ferromagnet cycling, all at 10-unit-cell thickness with high room-temperature stability. This paves the way for future work to establish the ultimate cycling frequency and endurance of such devices.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Appl Mater Interfaces Asunto de la revista: BIOTECNOLOGIA / ENGENHARIA BIOMEDICA Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Appl Mater Interfaces Asunto de la revista: BIOTECNOLOGIA / ENGENHARIA BIOMEDICA Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos