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Title: Antiferromagnetic defect structure in LaNi O 3 - δ single crystals

Abstract

The origins of the metal-insulator and magnetic transitions exhibited by perovskite rare-earth nickelates, RNiO3 (where R is a rare-earth element), remain open issues, with charge disproportionation, magnetic interactions, and lattice response across multiple length scales being among the many possible origins. Recently, growth of single crystals of LaNiO3, which is the only member of these compounds that remains metallic in its ground state, has been reported, opening a new chapter in the investigation of the perovskite nickelates. Here, using a combination of magnetometry, heat capacity, and neutron scattering on as-grown and purposely reduced LaNiO3-delta crystals, we show that both antiferromagnetic and ferromagnetic phases with a Neel temperature of similar to 152 K and a Curie temperature of similar to 225 K can be induced by reduction of the oxygen content. Transmission electron microscopy shows that these phases are characterized by ordered oxygen vacancy defect structures that exist as dilute secondary phases in as-grown crystals despite growth in partial oxygen pressures up to at least 130 bar. The demonstration of antiferromagnetism resulting from oxygen vacancy ordered structures implies that stoichiometry must be explicitly considered when interpreting the bulk properties of LaNiO3-(delta) single crystals; accordingly, the implications of our results for putativemore » oxygen-stoichiometric LaNiO3 are discussed.« less

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); USDOE
OSTI Identifier:
1461509
Alternate Identifier(s):
OSTI ID: 1441245
Grant/Contract Number:  
AC02-06CH11357; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 6; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English

Citation Formats

Wang, Bi-Xia, Rosenkranz, S., Rui, X., Zhang, Junjie, Ye, F., Zheng, H., Klie, R. F., Mitchell, J. F., and Phelan, D. Antiferromagnetic defect structure in LaNiO3-δ single crystals. United States: N. p., 2018. Web. doi:10.1103/PhysRevMaterials.2.064404.
Wang, Bi-Xia, Rosenkranz, S., Rui, X., Zhang, Junjie, Ye, F., Zheng, H., Klie, R. F., Mitchell, J. F., & Phelan, D. Antiferromagnetic defect structure in LaNiO3-δ single crystals. United States. doi:10.1103/PhysRevMaterials.2.064404.
Wang, Bi-Xia, Rosenkranz, S., Rui, X., Zhang, Junjie, Ye, F., Zheng, H., Klie, R. F., Mitchell, J. F., and Phelan, D. Fri . "Antiferromagnetic defect structure in LaNiO3-δ single crystals". United States. doi:10.1103/PhysRevMaterials.2.064404. https://www.osti.gov/servlets/purl/1461509.
@article{osti_1461509,
title = {Antiferromagnetic defect structure in LaNiO3-δ single crystals},
author = {Wang, Bi-Xia and Rosenkranz, S. and Rui, X. and Zhang, Junjie and Ye, F. and Zheng, H. and Klie, R. F. and Mitchell, J. F. and Phelan, D.},
abstractNote = {The origins of the metal-insulator and magnetic transitions exhibited by perovskite rare-earth nickelates, RNiO3 (where R is a rare-earth element), remain open issues, with charge disproportionation, magnetic interactions, and lattice response across multiple length scales being among the many possible origins. Recently, growth of single crystals of LaNiO3, which is the only member of these compounds that remains metallic in its ground state, has been reported, opening a new chapter in the investigation of the perovskite nickelates. Here, using a combination of magnetometry, heat capacity, and neutron scattering on as-grown and purposely reduced LaNiO3-delta crystals, we show that both antiferromagnetic and ferromagnetic phases with a Neel temperature of similar to 152 K and a Curie temperature of similar to 225 K can be induced by reduction of the oxygen content. Transmission electron microscopy shows that these phases are characterized by ordered oxygen vacancy defect structures that exist as dilute secondary phases in as-grown crystals despite growth in partial oxygen pressures up to at least 130 bar. The demonstration of antiferromagnetism resulting from oxygen vacancy ordered structures implies that stoichiometry must be explicitly considered when interpreting the bulk properties of LaNiO3-(delta) single crystals; accordingly, the implications of our results for putative oxygen-stoichiometric LaNiO3 are discussed.},
doi = {10.1103/PhysRevMaterials.2.064404},
journal = {Physical Review Materials},
number = 6,
volume = 2,
place = {United States},
year = {2018},
month = {6}
}

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    Works referencing / citing this record:

    High pO2 Floating Zone Crystal Growth of the Perovskite Nickelate PrNiO3
    journal, June 2019