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Colossal reversible conductivity switching by room-temperature oxygen-vacancy ordering in Aurivillius oxide films

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Abstract

Oxygen vacancies are central to the functionality of oxides, yet they typically exist as randomly distributed point defects, limiting the ability to precisely manipulate their collective behavior. Here, we report the room-temperature formation of a long-range-ordered oxygen-vacancy superstructure in single-crystalline Aurivillius-phase Bi2WO6 thin films via a mild nitrogen-plasma treatment. This structural transformation unlocks a colossal, reversible modulation of electrical conductivity by more than nine orders of magnitude, accompanied by a striking optical transition from transparent to black. Atomic-resolution imaging and spectroscopy reveal that the vacancies selectively order within the perovskite-like tungsten oxide layers, forming a coherent defect lattice that is absent in the pristine film. Oxygen-plasma treatment removes the vacancy superstructure and restores the initial state, whereas subsequent nitrogen-plasma treatment reconstructs it, enabling repeatable room-temperature switching between distinct structural, electronic and optical states. The phenomenon is also observed in another Aurivillius member, Bi2MoO6, suggesting its generality across the Aurivillius family. These findings establish a new paradigm for atomic-scale defect engineering - using gentle plasma chemistry to construct ordered defect lattices, opening avenues for reversible property modulation in complex oxides.

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BibTeX
@misc{zhou2026colossal,
  title = {{Colossal reversible conductivity switching by room-temperature oxygen-vacancy ordering in Aurivillius oxide films}},
  author = {Song Zhou and Songge Zhang and Lanting Shi and Ping Zhang and Na Li and Jiawei Huang and Bolin Meng and Chuangye Song and Shaoxiang Sheng and Yang Chai and Lede Xian and Jinxing Zheng and Guangyu Zhang and Kehui Wu},
  howpublished = {arXiv},
  year = {2026},
  month = sep,
  doi = {10.48550/arxiv.2609.02629},
  eprint = {2609.02629},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2609.02629},
}
RIS
TY  - UNPB
TI  - Colossal reversible conductivity switching by room-temperature oxygen-vacancy ordering in Aurivillius oxide films
AU  - Song Zhou
AU  - Songge Zhang
AU  - Lanting Shi
AU  - Ping Zhang
AU  - Na Li
AU  - Jiawei Huang
AU  - Bolin Meng
AU  - Chuangye Song
AU  - Shaoxiang Sheng
AU  - Yang Chai
AU  - Lede Xian
AU  - Jinxing Zheng
AU  - Guangyu Zhang
AU  - Kehui Wu
PY  - 2026
DA  - 2026/09/02
PB  - arXiv
DO  - 10.48550/arxiv.2609.02629
UR  - https://arxiv.org/abs/2609.02629
AB  - Oxygen vacancies are central to the functionality of oxides, yet they typically exist as randomly distributed point defects, limiting the ability to precisely manipulate their collective behavior. Here, we report the room-temperature formation of a long-range-ordered oxygen-vacancy superstructure in single-crystalline Aurivillius-phase Bi2WO6 thin films via a mild nitrogen-plasma treatment. This structural transformation unlocks a colossal, reversible modulation of electrical conductivity by more than nine orders of magnitude, accompanied by a striking optical transition from transparent to black. Atomic-resolution imaging and spectroscopy reveal that the vacancies selectively order within the perovskite-like tungsten oxide layers, forming a coherent defect lattice that is absent in the pristine film. Oxygen-plasma treatment removes the vacancy superstructure and restores the initial state, whereas subsequent nitrogen-plasma treatment reconstructs it, enabling repeatable room-temperature switching between distinct structural, electronic and optical states. The phenomenon is also observed in another Aurivillius member, Bi2MoO6, suggesting its generality across the Aurivillius family. These findings establish a new paradigm for atomic-scale defect engineering - using gentle plasma chemistry to construct ordered defect lattices, opening avenues for reversible property modulation in complex oxides.
ER  -