Tunable magnetic ordering through cation selection in entropic spinel oxides

Brianna Musicó, Quinton Wright, T. Zac Ward, Alexander Grutter, Elke Arenholz, Dustin Gilbert, David Mandrus, and Veerle Keppens
Phys. Rev. Materials 3, 104416 – Published 21 October 2019
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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 Fm3m 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.

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  • Received 18 June 2019

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

©2019 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Brianna Musicó1, Quinton Wright1, T. Zac Ward2, Alexander Grutter3, Elke Arenholz4, Dustin Gilbert1, David Mandrus1, and Veerle Keppens1,*

  • 1Joint Institute for Advanced Materials, Department of Materials Science and Engineering, University of Tennessee-Knoxville, Tennessee 37996-4545, USA
  • 2Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
  • 3NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899-6102, USA
  • 4Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA

  • *Corresponding author: vkeppens@utk.edu

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Vol. 3, Iss. 10 — October 2019

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