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

Title: Tunable magnetic ordering through cation selection in entropic spinel oxides

Journal Article · · Physical Review Materials
ORCiD logo [1];  [1]; ORCiD logo [2];  [3];  [4];  [1];  [1];  [1]
  1. Univ. of Tennessee, Knoxville, TN (United States). Joint Inst. of Neutron Science
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  3. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

Twelve multicomponent spinels, comprised of (Mg, Cr, Mn, Co, Fe, Ni, Cu, and/or Zn)(Cr,Fe,orAl)2O4, were prepared using solid state synthesis methods, resulting in nine homogenous, single phase samples with a Fm-3m structure, and three samples with multiple phases. Using dc magnetometry in conjunction with x-ray diffraction, scanning electron microscopy with energy dispersive x-ray spectroscopy, and x-ray absorption spectroscopy, the effects of multicomponent material design on the structural, magnetic, and chemical properties are explored. The ferritic spinel high-entropy oxide (HEO) samples show high-temperature ferrimagnetic transitions and both ferritic and chromium-based HEO spinel samples show evidence of low-temperature antiferromagnetic ordering. Blocking temperatures are evident in some samples and magnetic transition temperatures are reported. Constituent valence states and temperature dependent valence is described for the example case of (Mg0.2Fe0.2Co0.2Ni0.2Cu0.2)Cr2O4, including the unexpected presence of Cr4+, indicating a 2–4 type spinel configuration. Valence trends for two ferritic HEO spinels are also discussed. Some of these compositions are synthesized for the first time and this work provides an investigation into the magnetic properties of the novel class of cubic spinel multicomponent oxides showing interesting behavior that warrants further investigation.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1606826
Journal Information:
Physical Review Materials, Vol. 3, Issue 10; ISSN 2475-9953
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 59 works
Citation information provided by
Web of Science

References (33)

Entropy-stabilized oxides journal September 2015
Colossal dielectric constant in high entropy oxides journal March 2016
High-entropy fluorite oxides journal August 2018
Giant Enhancement of Exchange Coupling in Entropy-Stabilized Oxide Heterostructures journal October 2017
Characterization and magnetic properties of core/shell structured Fe/Au nanoparticles journal June 2004
Cation distribution and magnetic interactions in Zn-substituted CuFe2O4 ferrites journal August 2000
Synthesis and microstructure of the (Co,Cr,Fe,Mn,Ni) 3 O 4 high entropy oxide characterized by spinel structure journal April 2018
Ac susceptibility and magnetic interaction in Mg–Ni–Fe–O system journal December 2002
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides journal September 1976
Evolution of magnetic properties in the normal spinel solid solution Mg 1− x Cu x Cr 2 O 4 journal January 2012
Coexistence of ferrimagnetic and antiferromagnetic ordering in Fe-inverted zinc ferrite investigated by NMR journal February 2006
Rare earth and transition metal based entropy stabilised perovskite type oxides journal May 2018
Structural effects on the magnetic hyperthermia properties of iron oxide nanoparticles journal October 2016
Nanostructured High-Entropy Alloys with Multiple Principal Elements: Novel Alloy Design Concepts and Outcomes journal May 2004
GSAS-II : the genesis of a modern open-source all purpose crystallography software package journal March 2013
A new class of high-entropy perovskite oxides journal January 2018
Materials for Magnetic Recording [最近の磁気記録媒体] journal January 1969
Systematics of the spinel structure type journal January 1979
Single-crystal high entropy perovskite oxide epitaxial films journal June 2018
Cation Distribution and Magnetic Interactions in Zn-Substituted Fe(Cu)Fe2O4 Ferrites journal June 2012
Handbook of Advanced Magnetic Materials book January 2006
Magnetic phase evolution in the spinel compounds Zn 1− x Co x Cr 2 O 4 journal May 2009
A five-component entropy-stabilized fluorite oxide journal September 2018
Transition warming and cooling remanences in pyrrhotite and hematite journal September 2015
Magnetodielectric coupling in frustrated spin systems: the spinels MCr 2 O 4 (M = Mn, Co and Ni) journal February 2010
High-entropy oxides: An emerging prospect for magnetic rare-earth transition metal perovskites journal March 2019
FeCr 2 O 4 and CoCr 2 O 4 spinels: Multiferroicity in the collinear magnetic state? journal October 2011
Materials for Magnetic Recording journal August 1985
Structural and magnetic properties of ZnxCul.4−xMn0.4Fel.2O4 ferrites journal October 2005
Some physical and magnetic properties of Mg-Zn ferrite journal June 2003
Facile synthesis and ferrimagnetic property of spinel (CoCrFeMnNi)3O4 high-entropy oxide nanocrystalline powder journal October 2019
Magnetic phase evolution in the spinel compounds Zn$_{1-x}$Co$_x$Cr$_2$O$_4$ text January 2008
High entropy oxides: An emerging prospect for magnetic rare earth - transition metal perovskites text January 2019

Figures / Tables (10)