DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Long-Range Antiferromagnetic Order in a Rocksalt High Entropy Oxide

Abstract

We report for the first time the magnetic structure of the high entropy oxide (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O using neutron powder diffraction. This material exhibits a sluggish magnetic transition but possesses a long-range ordered antiferromagnetic ground state, as revealed by direct current and alternating current magnetic susceptibility, neutron diffraction, and spectroscopy. The magnetic propagation wavevector is k = (1/2, 1/2, 1/2) based on the cubic structure Fm3m, and the magnetic structure consists of ferromagnetic sheets in the (111) planes with spins antiparallel between two neighboring planes. Neutron spectroscopy reveals strong magnetic excitations at 100 K that survive up to room temperature. This work demonstrates that entropy-stabilized oxides represent a unique platform to study long-range magnetic order with an extreme chemical disorder.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [2]; ORCiD logo [1];  [2];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1513391
Alternate Identifier(s):
OSTI ID: 1529267
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 10; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Zhang, Junjie, Yan, Jiaqiang, Calder, Stuart A., Zheng, Qiang, McGuire, Michael A., Abernathy, Douglas L., Ren, Yang, Lapidus, Saul H., Page, Katharine L., Zheng, Hong, Freeland, John W., Budai, John D., and Hermann, Raphael P. Long-Range Antiferromagnetic Order in a Rocksalt High Entropy Oxide. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.9b00624.
Zhang, Junjie, Yan, Jiaqiang, Calder, Stuart A., Zheng, Qiang, McGuire, Michael A., Abernathy, Douglas L., Ren, Yang, Lapidus, Saul H., Page, Katharine L., Zheng, Hong, Freeland, John W., Budai, John D., & Hermann, Raphael P. Long-Range Antiferromagnetic Order in a Rocksalt High Entropy Oxide. United States. https://doi.org/10.1021/acs.chemmater.9b00624
Zhang, Junjie, Yan, Jiaqiang, Calder, Stuart A., Zheng, Qiang, McGuire, Michael A., Abernathy, Douglas L., Ren, Yang, Lapidus, Saul H., Page, Katharine L., Zheng, Hong, Freeland, John W., Budai, John D., and Hermann, Raphael P. Fri . "Long-Range Antiferromagnetic Order in a Rocksalt High Entropy Oxide". United States. https://doi.org/10.1021/acs.chemmater.9b00624. https://www.osti.gov/servlets/purl/1513391.
@article{osti_1513391,
title = {Long-Range Antiferromagnetic Order in a Rocksalt High Entropy Oxide},
author = {Zhang, Junjie and Yan, Jiaqiang and Calder, Stuart A. and Zheng, Qiang and McGuire, Michael A. and Abernathy, Douglas L. and Ren, Yang and Lapidus, Saul H. and Page, Katharine L. and Zheng, Hong and Freeland, John W. and Budai, John D. and Hermann, Raphael P.},
abstractNote = {We report for the first time the magnetic structure of the high entropy oxide (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O using neutron powder diffraction. This material exhibits a sluggish magnetic transition but possesses a long-range ordered antiferromagnetic ground state, as revealed by direct current and alternating current magnetic susceptibility, neutron diffraction, and spectroscopy. The magnetic propagation wavevector is k = (1/2, 1/2, 1/2) based on the cubic structure Fm3m, and the magnetic structure consists of ferromagnetic sheets in the (111) planes with spins antiparallel between two neighboring planes. Neutron spectroscopy reveals strong magnetic excitations at 100 K that survive up to room temperature. This work demonstrates that entropy-stabilized oxides represent a unique platform to study long-range magnetic order with an extreme chemical disorder.},
doi = {10.1021/acs.chemmater.9b00624},
journal = {Chemistry of Materials},
number = 10,
volume = 31,
place = {United States},
year = {2019},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 18 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

High‐Entropy Oxides: Fundamental Aspects and Electrochemical Properties
journal, March 2019

  • Sarkar, Abhishek; Wang, Qingsong; Schiele, Alexander
  • Advanced Materials, Vol. 31, Issue 26
  • DOI: 10.1002/adma.201806236

A critical review of high entropy alloys and related concepts
journal, January 2017


High-entropy alloy: challenges and prospects
journal, July 2016


Entropy-stabilized oxides
journal, September 2015

  • Rost, Christina M.; Sachet, Edward; Borman, Trent
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9485

Single-crystal high entropy perovskite oxide epitaxial films
journal, June 2018


Rare earth and transition metal based entropy stabilised perovskite type oxides
journal, May 2018


A new class of high-entropy perovskite oxides
journal, January 2018


Synthesis and microstructure of the (Co,Cr,Fe,Mn,Ni) 3 O 4 high entropy oxide characterized by spinel structure
journal, April 2018


Colossal dielectric constant in high entropy oxides
journal, March 2016

  • Bérardan, David; Franger, Sylvain; Dragoe, Diana
  • physica status solidi (RRL) - Rapid Research Letters, Vol. 10, Issue 4
  • DOI: 10.1002/pssr.201600043

Room temperature lithium superionic conductivity in high entropy oxides
journal, January 2016

  • Bérardan, D.; Franger, S.; Meena, A. K.
  • Journal of Materials Chemistry A, Vol. 4, Issue 24
  • DOI: 10.1039/C6TA03249D

High entropy oxides as anode material for Li-ion battery applications: A practical approach
journal, March 2019


High entropy oxides for reversible energy storage
journal, August 2018


Controlled Jahn-Teller distortion in (MgCoNiCuZn)O-based high entropy oxides
journal, May 2017


Local structure of the Mg x Ni x Co x Cu x Zn x O( x =0.2) entropy-stabilized oxide: An EXAFS study
journal, April 2017

  • Rost, Christina M.; Rak, Zsolt; Brenner, Donald W.
  • Journal of the American Ceramic Society, Vol. 100, Issue 6
  • DOI: 10.1111/jace.14756

Evidence for Jahn-Teller compression in the (Mg, Co, Ni, Cu, Zn)O entropy-stabilized oxide: A DFT study
journal, April 2018


Charge compensation and electrostatic transferability in three entropy-stabilized oxides: Results from density functional theory calculations
journal, September 2016

  • Rak, Zs.; Rost, C. M.; Lim, M.
  • Journal of Applied Physics, Vol. 120, Issue 9
  • DOI: 10.1063/1.4962135

Charge-Induced Disorder Controls the Thermal Conductivity of Entropy-Stabilized Oxides
journal, October 2018

  • Braun, Jeffrey L.; Rost, Christina M.; Lim, Mina
  • Advanced Materials, Vol. 30, Issue 51
  • DOI: 10.1002/adma.201805004

Giant Enhancement of Exchange Coupling in Entropy-Stabilized Oxide Heterostructures
journal, October 2017


High-entropy fluorite oxides
journal, August 2018


A five-component entropy-stabilized fluorite oxide
journal, September 2018


High-entropy oxides: An emerging prospect for magnetic rare-earth transition metal perovskites
journal, March 2019


The Nanoscale Ordered MAterials Diffractometer NOMAD at the Spallation Neutron Source SNS
journal, September 2012

  • Neuefeind, Jörg; Feygenson, Mikhail; Carruth, John
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 287
  • DOI: 10.1016/j.nimb.2012.05.037

PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals
journal, July 2007


Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source
journal, January 2012

  • Abernathy, D. L.; Stone, M. B.; Loguillo, M. J.
  • Review of Scientific Instruments, Vol. 83, Issue 1
  • DOI: 10.1063/1.3680104

DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data
journal, November 2009

  • Azuah, Richard Tumanjong; Kneller, Larry R.; Qiu, Yiming
  • Journal of Research of the National Institute of Standards and Technology, Vol. 114, Issue 6
  • DOI: 10.6028/jres.114.025

Large orbital polarization in a metallic square-planar nickelate
journal, June 2017

  • Zhang, Junjie; Botana, A. S.; Freeland, J. W.
  • Nature Physics, Vol. 13, Issue 9
  • DOI: 10.1038/nphys4149

Evolution of electronic structure across the rare-earth RNiO3 series
journal, April 2016

  • Freeland, John W.; van Veenendaal, Michel; Chakhalian, Jak
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 208
  • DOI: 10.1016/j.elspec.2015.07.006

Electronic structure and metal-insulator transition in LaNiO 3 δ
journal, March 2002


Strain Control of Oxygen Vacancies in Epitaxial Strontium Cobaltite Films
journal, January 2016

  • Petrie, Jonathan R.; Mitra, Chandrima; Jeen, Hyoungjeen
  • Advanced Functional Materials, Vol. 26, Issue 10
  • DOI: 10.1002/adfm.201504868

Electronic structure and magnetic states in La 1 x Sr x CoO 3 studied by photoemission and x-ray-absorption spectroscopy
journal, July 1997


On the homogeneity of high entropy oxides: An investigation at the atomic scale
journal, June 2019


Melting of Quasi-Two-Dimensional Charge Stripes in La 5 / 3 Sr 1 / 3 NiO 4
journal, September 1997


A suite-level review of the neutron powder diffraction instruments at Oak Ridge National Laboratory
journal, September 2018

  • Calder, S.; An, K.; Boehler, R.
  • Review of Scientific Instruments, Vol. 89, Issue 9
  • DOI: 10.1063/1.5033906

The high-resolution powder diffractometer at the high flux isotope reactor
journal, March 2010


Indexing magnetic structures and crystallographic distortions from powder diffraction: Brillouin zone indexing
journal, September 2009


Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993


Magnetic Structures of MnO, FeO, CoO, and NiO
journal, June 1958


Magnetic phase diagrams of diluted fcc antiferromagnets Co p Mg 1 p O and Eu p Sr 1 p Te
journal, April 1988


Magnetic Phase Diagram of (Ni1−xMgx)O Solid Solutions
journal, March 1991

  • Menshikov, A. Z.; Dorofeev, Yu. A.; Klimenko, A. G.
  • physica status solidi (b), Vol. 164, Issue 1
  • DOI: 10.1002/pssb.2221640130

Superexchange interaction and symmetry properties of electron orbitals
journal, July 1959


An interpretation of the magnetic properties of the perovskite-type mixed crystals La1−xSrxCoO3−λ
journal, August 1958


Origin of antiferromagnetism in CoO: A density functional theory study
journal, April 2010

  • Deng, Hui-Xiong; Li, Jingbo; Li, Shu-Shen
  • Applied Physics Letters, Vol. 96, Issue 16
  • DOI: 10.1063/1.3402772

Magnetic Ordering in Polycrystalline NixZn1?xO Solid Solutions
journal, April 2000


Deformations in the Crystal Structures of Anti-ferromagnetic Compounds
journal, September 1950

  • Greenwald, Selma; Smart, J. Samuel
  • Nature, Vol. 166, Issue 4221
  • DOI: 10.1038/166523a0

A neutron diffraction study of the structure of the antiferromagnet CopNi1−pO
journal, January 1979

  • Battle, P. D.; Cheetham, A. K.; Gehring, G. A.
  • Journal of Applied Physics, Vol. 50, Issue B11
  • DOI: 10.1063/1.326850

Magnetoelastic coupling forbidden by time-reversal symmetry: Spin-direction-dependent magnetoelastic coupling on MnO, CoO, and NiO
journal, February 2016


Optical spectroscopy in CoO: Phononic, electric, and magnetic excitation spectrum within the charge-transfer gap
journal, December 2008


Works referencing / citing this record:

Magnetic anisotropy in single-crystal high-entropy perovskite oxide La ( C r 0.2 M n 0.2 F e 0.2 C o 0.2 N i 0.2 ) O 3 films
journal, January 2020


Magnetic frustration control through tunable stereochemically driven disorder in entropy-stabilized oxides
journal, October 2019


High-entropy ceramics
journal, February 2020


Photocatalytic hydrogen evolution on a high-entropy oxide
journal, January 2020

  • Edalati, Parisa; Wang, Qing; Razavi-Khosroshahi, Hadi
  • Journal of Materials Chemistry A, Vol. 8, Issue 7
  • DOI: 10.1039/c9ta12846h