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Title: Redox Gating for Colossal Carrier Modulation and Unique Phase Control

Abstract

Abstract Redox gating, a novel approach distinct from conventional electrolyte gating, combines reversible redox functionalities with common ionic electrolyte moieties to engineer charge transport, enabling power‐efficient electronic phase control. This study achieves a colossal sheet carrier density modulation beyond 10 16 cm −2 , sustainable over thousands of cycles, all within the sub‐volt regime for functional oxide thin films. The key advantage of this method lies in the controlled injection of a large quantity of carriers from the electrolyte into the channel material without the deleterious effects associated with traditional electrolyte gating processes such as the production of ionic defects or intercalated species. The redox gating approach offers a simple and practical means of decoupling electrical and structural phase transitions, enabling the isostructural metal‐insulator transition and improved device endurance. The versatility of redox gating extends across multiple materials, irrespective of their crystallinity, crystallographic orientation, or carrier type (n‐ or p‐type). This inclusivity encompasses functional heterostructures and low‐dimensional quantum materials composed of sustainable elements, highlighting the broad applicability and potential of the technique in electronic devices.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [4];  [5]; ORCiD logo [6]; ORCiD logo [7]; ORCiD logo [8]; ORCiD logo [9]; ORCiD logo [8]
  1. Materials Science Division Argonne National Laboratory Lemont IL 60439 USA, Center for Molecular Engineering Argonne National Laboratory Lemont IL 60439 USA
  2. Materials Science Division Argonne National Laboratory Lemont IL 60439 USA, Department of Physics University at Buffalo SUNY Buffalo NY 14260 USA
  3. Materials Science Division Argonne National Laboratory Lemont IL 60439 USA, Center for Molecular Engineering Argonne National Laboratory Lemont IL 60439 USA, X‐ray Science Division Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA
  4. Materials Science Division Argonne National Laboratory Lemont IL 60439 USA
  5. Department of Chemistry and the James Franck Institute University of Chicago Chicago IL 60637 USA
  6. Center for Nanoscale Materials Nanoscience and Technology Division Argonne National Laboratory Lemont IL 60439 USA
  7. National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230029 China
  8. Materials Science Division Argonne National Laboratory Lemont IL 60439 USA, Center for Molecular Engineering Argonne National Laboratory Lemont IL 60439 USA, Pritzker School of Molecular Engineering University of Chicago Chicago IL 60637 USA
  9. X‐ray Science Division Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
2281256
Alternate Identifier(s):
OSTI ID: 2281257
Resource Type:
Published Article
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Name: Advanced Materials Journal Volume: 36 Journal Issue: 16; Journal ID: ISSN 0935-9648
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Zhang, Le, Liu, Changjiang, Cao, Hui, Erwin, Andrew J., Fong, Dillon D., Bhattacharya, Anand, Yu, Luping, Stan, Liliana, Zou, Chongwen, Tirrell, Matthew V., Zhou, Hua, and Chen, Wei. Redox Gating for Colossal Carrier Modulation and Unique Phase Control. Germany: N. p., 2024. Web. doi:10.1002/adma.202308871.
Zhang, Le, Liu, Changjiang, Cao, Hui, Erwin, Andrew J., Fong, Dillon D., Bhattacharya, Anand, Yu, Luping, Stan, Liliana, Zou, Chongwen, Tirrell, Matthew V., Zhou, Hua, & Chen, Wei. Redox Gating for Colossal Carrier Modulation and Unique Phase Control. Germany. https://doi.org/10.1002/adma.202308871
Zhang, Le, Liu, Changjiang, Cao, Hui, Erwin, Andrew J., Fong, Dillon D., Bhattacharya, Anand, Yu, Luping, Stan, Liliana, Zou, Chongwen, Tirrell, Matthew V., Zhou, Hua, and Chen, Wei. Sun . "Redox Gating for Colossal Carrier Modulation and Unique Phase Control". Germany. https://doi.org/10.1002/adma.202308871.
@article{osti_2281256,
title = {Redox Gating for Colossal Carrier Modulation and Unique Phase Control},
author = {Zhang, Le and Liu, Changjiang and Cao, Hui and Erwin, Andrew J. and Fong, Dillon D. and Bhattacharya, Anand and Yu, Luping and Stan, Liliana and Zou, Chongwen and Tirrell, Matthew V. and Zhou, Hua and Chen, Wei},
abstractNote = {Abstract Redox gating, a novel approach distinct from conventional electrolyte gating, combines reversible redox functionalities with common ionic electrolyte moieties to engineer charge transport, enabling power‐efficient electronic phase control. This study achieves a colossal sheet carrier density modulation beyond 10 16 cm −2 , sustainable over thousands of cycles, all within the sub‐volt regime for functional oxide thin films. The key advantage of this method lies in the controlled injection of a large quantity of carriers from the electrolyte into the channel material without the deleterious effects associated with traditional electrolyte gating processes such as the production of ionic defects or intercalated species. The redox gating approach offers a simple and practical means of decoupling electrical and structural phase transitions, enabling the isostructural metal‐insulator transition and improved device endurance. The versatility of redox gating extends across multiple materials, irrespective of their crystallinity, crystallographic orientation, or carrier type (n‐ or p‐type). This inclusivity encompasses functional heterostructures and low‐dimensional quantum materials composed of sustainable elements, highlighting the broad applicability and potential of the technique in electronic devices.},
doi = {10.1002/adma.202308871},
journal = {Advanced Materials},
number = 16,
volume = 36,
place = {Germany},
year = {Sun Jan 14 00:00:00 EST 2024},
month = {Sun Jan 14 00:00:00 EST 2024}
}

Journal Article:
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https://doi.org/10.1002/adma.202308871

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