Carrier localization in perovskite nickelates from oxygen vacancies

Point defects, such as oxygen vacancies, control the physical properties of complex oxides, relevant in active areas of research from superconductivity to resistive memory to catalysis. In most oxide semiconductors, electrons that are associated with oxygen vacancies occupy the conduction band, lead...

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Main Authors: Kotiuga, Michele, Zhang, Zhen, Li, Jiarui, Rodolakis, Fanny, Zhou, Hua, Sutarto, Ronny, He, Feizhou, Wang, Qi, Sun, Yifei, Wang, Ying, Aghamiri, Neda Alsadat, Hancock, Steven Bennett, Rokhinson, Leonid P, Landau, David P, Abate, Yohannes, Freeland, John W, Comin, Riccardo, Ramanathan, Shriram, Rabe, Karin M
Other Authors: Massachusetts Institute of Technology. Department of Physics
Format: Article
Language:English
Published: National Academy of Sciences 2020
Online Access:https://hdl.handle.net/1721.1/127812
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author Kotiuga, Michele
Zhang, Zhen
Li, Jiarui
Rodolakis, Fanny
Zhou, Hua
Sutarto, Ronny
He, Feizhou
Wang, Qi
Sun, Yifei
Wang, Ying
Aghamiri, Neda Alsadat
Hancock, Steven Bennett
Rokhinson, Leonid P
Landau, David P
Abate, Yohannes
Freeland, John W
Comin, Riccardo
Ramanathan, Shriram
Rabe, Karin M
author2 Massachusetts Institute of Technology. Department of Physics
author_facet Massachusetts Institute of Technology. Department of Physics
Kotiuga, Michele
Zhang, Zhen
Li, Jiarui
Rodolakis, Fanny
Zhou, Hua
Sutarto, Ronny
He, Feizhou
Wang, Qi
Sun, Yifei
Wang, Ying
Aghamiri, Neda Alsadat
Hancock, Steven Bennett
Rokhinson, Leonid P
Landau, David P
Abate, Yohannes
Freeland, John W
Comin, Riccardo
Ramanathan, Shriram
Rabe, Karin M
author_sort Kotiuga, Michele
collection MIT
description Point defects, such as oxygen vacancies, control the physical properties of complex oxides, relevant in active areas of research from superconductivity to resistive memory to catalysis. In most oxide semiconductors, electrons that are associated with oxygen vacancies occupy the conduction band, leading to an increase in the electrical conductivity. Here we demonstrate, in contrast, that in the correlatedelectron perovskite rare-earth nickelates, RNiO3 (R is a rare-earth element such as Sm or Nd), electrons associated with oxygen vacancies strongly localize, leading to a dramatic decrease in the electrical conductivity by several orders of magnitude. This unusual behavior is found to stem from the combination of crystal field splitting and filling-controlled Mott-Hubbard electron-electron correlations in the Ni 3d orbitals. Furthermore, we show the distribution of oxygen vacancies in NdNiO3 can be controlled via an electric field, leading to analog resistance switching behavior. This study demonstrates the potential of nickelates as testbeds to better understand emergent physics in oxide heterostructures as well as candidate systems in the emerging fields of artificial intelligence.
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spelling mit-1721.1/1278122022-09-23T14:23:22Z Carrier localization in perovskite nickelates from oxygen vacancies Kotiuga, Michele Zhang, Zhen Li, Jiarui Rodolakis, Fanny Zhou, Hua Sutarto, Ronny He, Feizhou Wang, Qi Sun, Yifei Wang, Ying Aghamiri, Neda Alsadat Hancock, Steven Bennett Rokhinson, Leonid P Landau, David P Abate, Yohannes Freeland, John W Comin, Riccardo Ramanathan, Shriram Rabe, Karin M Massachusetts Institute of Technology. Department of Physics Point defects, such as oxygen vacancies, control the physical properties of complex oxides, relevant in active areas of research from superconductivity to resistive memory to catalysis. In most oxide semiconductors, electrons that are associated with oxygen vacancies occupy the conduction band, leading to an increase in the electrical conductivity. Here we demonstrate, in contrast, that in the correlatedelectron perovskite rare-earth nickelates, RNiO3 (R is a rare-earth element such as Sm or Nd), electrons associated with oxygen vacancies strongly localize, leading to a dramatic decrease in the electrical conductivity by several orders of magnitude. This unusual behavior is found to stem from the combination of crystal field splitting and filling-controlled Mott-Hubbard electron-electron correlations in the Ni 3d orbitals. Furthermore, we show the distribution of oxygen vacancies in NdNiO3 can be controlled via an electric field, leading to analog resistance switching behavior. This study demonstrates the potential of nickelates as testbeds to better understand emergent physics in oxide heterostructures as well as candidate systems in the emerging fields of artificial intelligence. National Science Foundation (Grant 1751739) 2020-10-05T21:42:26Z 2020-10-05T21:42:26Z 2019-10 2019-06 2020-09-22T18:21:25Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/127812 Kotiuga, Michele et al. "Carrier localization in perovskite nickelates from oxygen vacancies." Proceedings of the National Academy of Sciences 116, 44 (October 2019): 21992-21997 © 2019 National Academy of Sciences en https://dx.doi.org/10.1073/PNAS.1910490116 Proceedings of the National Academy of Sciences Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf National Academy of Sciences PNAS
spellingShingle Kotiuga, Michele
Zhang, Zhen
Li, Jiarui
Rodolakis, Fanny
Zhou, Hua
Sutarto, Ronny
He, Feizhou
Wang, Qi
Sun, Yifei
Wang, Ying
Aghamiri, Neda Alsadat
Hancock, Steven Bennett
Rokhinson, Leonid P
Landau, David P
Abate, Yohannes
Freeland, John W
Comin, Riccardo
Ramanathan, Shriram
Rabe, Karin M
Carrier localization in perovskite nickelates from oxygen vacancies
title Carrier localization in perovskite nickelates from oxygen vacancies
title_full Carrier localization in perovskite nickelates from oxygen vacancies
title_fullStr Carrier localization in perovskite nickelates from oxygen vacancies
title_full_unstemmed Carrier localization in perovskite nickelates from oxygen vacancies
title_short Carrier localization in perovskite nickelates from oxygen vacancies
title_sort carrier localization in perovskite nickelates from oxygen vacancies
url https://hdl.handle.net/1721.1/127812
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