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Title: Sudden Collapse of Magnetic Order in Oxygen-Deficient Nickelate Films

Abstract

Antiferromagnetic order is a common and robust ground state in the parent (undoped) phase of several strongly correlated electron systems. The progressive weakening of antiferromagnetic correlations upon doping paves the way for a variety of emergent many-electron phenomena including unconventional superconductivity, colossal magnetoresistance, and collective charge-spin-orbital ordering. In this study, we explored the use of oxygen stoichiometry as an alternative pathway to modify the coupled magnetic and electronic ground state in the family of rare earth nickelates ( RENiO3 - x). Using a combination of x-ray spectroscopy and resonant soft x-ray magnetic scattering, we find that, while oxygen vacancies rapidly alter the electronic configuration within the Ni and O orbital manifolds, antiferromagnetic order is remarkably robust to substantial levels of carrier doping, only to suddenly collapse beyond 0.21 e - / Ni without an accompanying structural transition. Our work demonstrates that ordered magnetism in RENiO3 - x is mostly insensitive to carrier doping up to significant levels unseen in other transition-metal oxides. The sudden collapse of ordered magnetism upon oxygen removal may provide a new mechanism for solid-state magnetoionic switching and new applications in antiferromagnetic spintronics.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [5];  [6];  [6]; ORCiD logo [6];  [3];  [4];  [3];  [6]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Univ. of Saskatchewan, Saskatoon, SK (Canada); Univ. of British Columbia, Vancouver, BC (Canada)
  3. Purdue Univ., West Lafayette, IN (United States)
  4. Canadian Light Sources, Inc., Saskatoon, SK (Canada)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR); Natural Sciences and Engineering Research Council of Canada (NSERC); National Science Foundation (NSF)
OSTI Identifier:
1797364
Report Number(s):
BNL-221672-2021-JAAM
Journal ID: ISSN 0031-9007; TRN: US2212336
Grant/Contract Number:  
SC0012704; FA9550-19-1-0351; FA9550-19-1-0063; 1751739
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 126; Journal Issue: 18; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Li, Jiarui, Green, Robert J., Zhang, Zhen, Sutarto, Ronny, Sadowski, Jerzy T., Zhu, Zhihai, Zhang, Grace, Zhou, Da, Sun, Yifei, He, Feizhou, Ramanathan, Shriram, and Comin, Riccardo. Sudden Collapse of Magnetic Order in Oxygen-Deficient Nickelate Films. United States: N. p., 2021. Web. doi:10.1103/physrevlett.126.187602.
Li, Jiarui, Green, Robert J., Zhang, Zhen, Sutarto, Ronny, Sadowski, Jerzy T., Zhu, Zhihai, Zhang, Grace, Zhou, Da, Sun, Yifei, He, Feizhou, Ramanathan, Shriram, & Comin, Riccardo. Sudden Collapse of Magnetic Order in Oxygen-Deficient Nickelate Films. United States. https://doi.org/10.1103/physrevlett.126.187602
Li, Jiarui, Green, Robert J., Zhang, Zhen, Sutarto, Ronny, Sadowski, Jerzy T., Zhu, Zhihai, Zhang, Grace, Zhou, Da, Sun, Yifei, He, Feizhou, Ramanathan, Shriram, and Comin, Riccardo. Thu . "Sudden Collapse of Magnetic Order in Oxygen-Deficient Nickelate Films". United States. https://doi.org/10.1103/physrevlett.126.187602. https://www.osti.gov/servlets/purl/1797364.
@article{osti_1797364,
title = {Sudden Collapse of Magnetic Order in Oxygen-Deficient Nickelate Films},
author = {Li, Jiarui and Green, Robert J. and Zhang, Zhen and Sutarto, Ronny and Sadowski, Jerzy T. and Zhu, Zhihai and Zhang, Grace and Zhou, Da and Sun, Yifei and He, Feizhou and Ramanathan, Shriram and Comin, Riccardo},
abstractNote = {Antiferromagnetic order is a common and robust ground state in the parent (undoped) phase of several strongly correlated electron systems. The progressive weakening of antiferromagnetic correlations upon doping paves the way for a variety of emergent many-electron phenomena including unconventional superconductivity, colossal magnetoresistance, and collective charge-spin-orbital ordering. In this study, we explored the use of oxygen stoichiometry as an alternative pathway to modify the coupled magnetic and electronic ground state in the family of rare earth nickelates ( RENiO3 - x). Using a combination of x-ray spectroscopy and resonant soft x-ray magnetic scattering, we find that, while oxygen vacancies rapidly alter the electronic configuration within the Ni and O orbital manifolds, antiferromagnetic order is remarkably robust to substantial levels of carrier doping, only to suddenly collapse beyond 0.21 e - / Ni without an accompanying structural transition. Our work demonstrates that ordered magnetism in RENiO3 - x is mostly insensitive to carrier doping up to significant levels unseen in other transition-metal oxides. The sudden collapse of ordered magnetism upon oxygen removal may provide a new mechanism for solid-state magnetoionic switching and new applications in antiferromagnetic spintronics.},
doi = {10.1103/physrevlett.126.187602},
journal = {Physical Review Letters},
number = 18,
volume = 126,
place = {United States},
year = {Thu May 06 00:00:00 EDT 2021},
month = {Thu May 06 00:00:00 EDT 2021}
}

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