Critical ionic transport across an oxygen-vacancy ordering transition

Ji Soo Lim, Ho-Hyun Nahm, Marco Campanini, Jounghee Lee, Yong-Jin Kim, Heung-Sik Park, Jeonghun Suh, Jun Jung, Yongsoo Yang, Tae Yeong Koo, Marta D. Rossell (), Yong-Hyun Kim () and Chan-Ho Yang ()
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Ji Soo Lim: Korea Advanced Institute of Science and Technology (KAIST)
Ho-Hyun Nahm: Korea Advanced Institute of Science and Technology (KAIST)
Marco Campanini: Electron Microscopy Center, Empa
Jounghee Lee: Korea Advanced Institute of Science and Technology (KAIST)
Yong-Jin Kim: Korea Advanced Institute of Science and Technology (KAIST)
Heung-Sik Park: Korea Advanced Institute of Science and Technology (KAIST)
Jeonghun Suh: Korea Advanced Institute of Science and Technology (KAIST)
Jun Jung: Korea Advanced Institute of Science and Technology (KAIST)
Yongsoo Yang: Korea Advanced Institute of Science and Technology (KAIST)
Tae Yeong Koo: Pohang Accelerator Laboratory, POSTECH
Marta D. Rossell: Electron Microscopy Center, Empa
Yong-Hyun Kim: Korea Advanced Institute of Science and Technology (KAIST)
Chan-Ho Yang: Korea Advanced Institute of Science and Technology (KAIST)

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Phase transition points can be used to critically reduce the ionic migration activation energy, which is important for realizing high-performance electrolytes at low temperatures. Here, we demonstrate a route toward low-temperature thermionic conduction in solids, by exploiting the critically lowered activation energy associated with oxygen transport in Ca-substituted bismuth ferrite (Bi1-xCaxFeO3-δ) films. Our demonstration relies on the finding that a compositional phase transition occurs by varying Ca doping ratio across xCa ≃ 0.45 between two structural phases with oxygen-vacancy channel ordering along or crystal axis, respectively. Regardless of the atomic-scale irregularity in defect distribution at the doping ratio, the activation energy is largely suppressed to 0.43 eV, compared with ~0.9 eV measured in otherwise rigid phases. From first-principles calculations, we propose that the effective short-range attraction between two positively charged oxygen vacancies sharing lattice deformation not only forms the defect orders but also suppresses the activation energy through concerted hopping.

Date: 2022
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DOI: 10.1038/s41467-022-32826-8

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