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

Tunable magnetic ordering through cation selection in entropic spinel oxides

Journal Article · Mon Oct 21 00:00:00 EDT 2019 · Physical Review Materials

DOI:https://doi.org/10.1103/PhysRevMaterials.3.104416· OSTI ID:1606826

^[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)

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.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1606826

Journal Information:: Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 10 Vol. 3; ISSN PRMHAR; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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