Carrier localization in perovskite nickelates from oxygen vacancies

doi:10.1073/pnas.1910490116

Title: Carrier localization in perovskite nickelates from oxygen vacancies

Abstract

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 correlated-electron perovskite rare-earth nickelates, R NiO ₃ ( 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 3 d orbitals. Furthermore, we show the distribution of oxygen vacancies in NdNiO ₃ 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.

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.

Publication Date:: 2019-10-14

Sponsoring Org.:: USDOE

OSTI Identifier:: 1570476

Grant/Contract Number:: SC0008630

Resource Type:: Published Article

Journal Name:: Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:: Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 116 Journal Issue: 44; Journal ID: ISSN 0027-8424

Publisher:: Proceedings of the National Academy of Sciences

Country of Publication:: United States

Language:: English

Citation Formats


                    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, and Rabe, Karin M. Carrier localization in perovskite nickelates from oxygen vacancies.  United States: N. p., 2019. 
        Web.  doi:10.1073/pnas.1910490116.

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                    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.  United States.  doi:10.1073/pnas.1910490116.

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                    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, and Rabe, Karin M. Mon .  
        "Carrier localization in perovskite nickelates from oxygen vacancies".  United States.  doi:10.1073/pnas.1910490116.

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@article{osti_1570476,

  title        = {Carrier localization in perovskite nickelates from oxygen vacancies},

  author       = {Kotiuga, Michele and Zhang, Zhen and Li, Jiarui and Rodolakis, Fanny and Zhou, Hua and Sutarto, Ronny and He, Feizhou and Wang, Qi and Sun, Yifei and Wang, Ying and Aghamiri, Neda Alsadat and Hancock, Steven Bennett and Rokhinson, Leonid P. and Landau, David P. and Abate, Yohannes and Freeland, John W. and Comin, Riccardo and Ramanathan, Shriram and Rabe, Karin M.},

  abstractNote = {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 correlated-electron perovskite rare-earth nickelates, R NiO 3 ( 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 3 d orbitals. Furthermore, we show the distribution of oxygen vacancies in NdNiO 3 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.},

  doi          = {10.1073/pnas.1910490116},

  journal      = {Proceedings of the National Academy of Sciences of the United States of America},

  number       = 44,

  volume       = 116,

  place        = {United States},

  year         = {2019},

  month        = {10}

}

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DOI: 10.1073/pnas.1910490116

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Works referenced in this record:

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Title: Carrier localization in perovskite nickelates from oxygen vacancies

Abstract

Citation Formats

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Projector augmented-wave method journal, December 1994

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Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

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