Tunable magnetic ordering through cation selection in entropic spinel oxides

Musico, Brianna L.; Wright, Quinton; Ward, Zac; Grutter, Alexander; Arenholz, Elke; Gilbert, Dustin; Mandrus, David; Keppens, Veerle

doi:10.1103/PhysRevMaterials.3.104416

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

Abstract

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 (Mg_0.2Fe_0.2Co_0.2Ni_0.2Cu_0.2)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.

Authors:

^[1]; Wright, Quinton ^[1];

^[2]; Grutter, Alexander ^[3]; Arenholz, Elke ^[4]; Gilbert, Dustin ^[1]; Mandrus, David ^[1]; Keppens, Veerle ^[1]

Univ. of Tennessee, Knoxville, TN (United States). Joint Inst. of Neutron Science
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

Publication Date:: Mon Oct 21 00:00:00 EDT 2019

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1606826

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Materials

Additional Journal Information:: Journal Volume: 3; Journal Issue: 10; Journal ID: ISSN 2475-9953

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Magnetic phase transitions; Magnetism; Polycrystalline materials; Spinel; Magnetization measurements; X-ray absorption spectroscopy; X-ray magnetic linear dichroism

Citation Formats


                    Musico, Brianna L., Wright, Quinton, Ward, Zac, Grutter, Alexander, Arenholz, Elke, Gilbert, Dustin, Mandrus, David, and Keppens, Veerle. Tunable magnetic ordering through cation selection in entropic spinel oxides.  United States: N. p., 2019. 
Web.  doi:10.1103/PhysRevMaterials.3.104416.

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                    Musico, Brianna L., Wright, Quinton, Ward, Zac, Grutter, Alexander, Arenholz, Elke, Gilbert, Dustin, Mandrus, David, & Keppens, Veerle. Tunable magnetic ordering through cation selection in entropic spinel oxides.  United States.  https://doi.org/10.1103/PhysRevMaterials.3.104416

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                    Musico, Brianna L., Wright, Quinton, Ward, Zac, Grutter, Alexander, Arenholz, Elke, Gilbert, Dustin, Mandrus, David, and Keppens, Veerle. Mon .  
"Tunable magnetic ordering through cation selection in entropic spinel oxides".  United States.  https://doi.org/10.1103/PhysRevMaterials.3.104416.  https://www.osti.gov/servlets/purl/1606826.

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@article{osti_1606826,

  title        = {Tunable magnetic ordering through cation selection in entropic spinel oxides},

  author       = {Musico, Brianna L. and Wright, Quinton and Ward, Zac and Grutter, Alexander and Arenholz, Elke and Gilbert, Dustin and Mandrus, David and Keppens, Veerle},

  abstractNote = {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.},

  doi          = {10.1103/PhysRevMaterials.3.104416},

  journal      = {Physical Review Materials},

  number       = 10,

  volume       = 3,

  place        = {United States},

  year         = {Mon Oct 21 00:00:00 EDT 2019},

  month        = {Mon Oct 21 00:00:00 EDT 2019}

}

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https://doi.org/10.1103/PhysRevMaterials.3.104416

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Figures / Tables:

Figure 1: X-ray diffraction for single phase HEO spinel compositions that are a) chromium based, b) iron based and c) aluminum based compared with ICSD reference patterns showing single phase spinel $Fd$-$3m$ structure.

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

Abstract

Citation Formats

Figures / Tables:

Entropy-stabilized oxides journal, September 2015

Colossal dielectric constant in high entropy oxides journal, March 2016

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Evolution of magnetic properties in the normal spinel solid solution Mg 1− x Cu x Cr 2 O 4 journal, January 2012

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

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Cation Distribution and Magnetic Interactions in Zn-Substituted Fe(Cu)Fe2O4 Ferrites journal, June 2012

Handbook of Advanced Magnetic Materials book, January 2006

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

Transition warming and cooling remanences in pyrrhotite and hematite journal, September 2015

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Ac susceptibility and magnetic interaction in Mg–Ni–Fe–O system
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Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
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Evolution of magnetic properties in the normal spinel solid solution Mg _{1− x} Cu _x Cr ₂ O ₄
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Cation Distribution and Magnetic Interactions in Zn-Substituted Fe(Cu)Fe2O4 Ferrites
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Magnetic phase evolution in the spinel compounds Zn _{1− x} Co _x Cr ₂ O ₄
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