Studies on the structure and the magnetic properties of high-entropy spinel oxide (MgMnFeCoNi)Al2O4

Evan Krysko; Lujin Min; Yu Wang; Na Zhang; John P. Barber; Gabriela E. Niculescu; Joshua T. Wright; Fankang Li; Kaleb Burrage; Masaaki Matsuda; Robert A. Robinson; Qiang Zhang; Rowan Katzbaer; Raymond Schaak; Mauricio Terrones; Christina M. Rost; Zhiqiang Mao

doi:10.1063/5.0161401

Studies on the structure and the magnetic properties of high-entropy spinel oxide (MgMnFeCoNi)Al₂O₄

Evan Krysko, Lujin Min, Yu Wang, Na Zhang, John P. Barber, Gabriela E. Niculescu, Joshua T. Wright, Fankang Li, Kaleb Burrage, Masaaki Matsuda, Robert A. Robinson, Qiang Zhang, Rowan Katzbaer, Raymond Schaak, Mauricio Terrones, Christina M. Rost, Zhiqiang Mao

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Abstract

The study of high-entropy materials has attracted enormous interest since they could show new functional properties that are not observed in their related parent phases. Here, we report single crystal growth, structure, thermal transport, and magnetic property studies on a novel high-entropy oxide with the spinel structure (MgMnFeCoNi)Al₂O₄. We have successfully grown high-quality single crystals of this high-entropy oxide using the optical floating zone growth technique for the first time. The sample was confirmed to be a phase pure high-entropy oxide using x-ray diffraction and energy-dispersive spectroscopy. Through magnetization measurements, we found (MgMnFeCoNi)Al₂O₄ exhibits a cluster spin glass state, though the parent phases show either antiferromagnetic ordering or spin glass states. Furthermore, we also found that (MgMnFeCoNi)Al₂O₄ has much greater thermal expansion than its CoAl₂O₄ parent compound using high resolution neutron Larmor diffraction. We further investigated the structure of this high-entropy material via Raman spectroscopy and extended x-ray absorption fine structure spectroscopy (EXAFS) measurements. From Raman spectroscopy measurements, we observed (MgMnFeCoNi)Al₂O₄ to display a combination of the active Raman modes in its parent compounds with the modes shifted and significantly broadened. This result, together with the varying bond lengths probed by EXAFS, reveals severe local lattice distortions in this high-entropy phase. Additionally, we found a substantial decrease in thermal conductivity and suppression of the low temperature thermal conductivity peak in (MgMnFeCoNi)Al₂O₄, consistent with the increased lattice defects and strain. These findings advance the understanding of the dependence of thermal expansion and transport on the lattice distortions in high-entropy materials.

Original language	English
Article number	101123
Journal	APL Materials
Volume	11
Issue number	10
DOIs	https://doi.org/10.1063/5.0161401
State	Published - Oct 1 2023

Funding

We would like to acknowledge George Kotsonis for the valuable discussion. This work was primarily supported by the Materials Research Science and Engineering Centers (MRSEC) under Award No. DMR 2011839. E.K. and Z.M. also acknowledge the support provided by the U.S. National Science Foundation under Grant No. DMR 2211327. A portion of this research used resources at the High Flux Isotope Reactor, Department of Energy Office of Science User Facilities operated by Oak Ridge National Laboratory. The development of the Larmor diffraction technique was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Early Career Research Program Award (No. KC0402010), under Contract No. DE-AC05-00OR22725. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. This research used resources from the Advanced Photon Source, a U.S. Department of Energy Office of Science User Facility operated for the Department of Energy Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. We would like to acknowledge George Kotsonis for the valuable discussion. This work was primarily supported by the Materials Research Science and Engineering Centers (MRSEC) under Award No. DMR 2011839. E.K. and Z.M. also acknowledge the support provided by the U.S. National Science Foundation under Grant No. DMR 2211327. A portion of this research used resources at the High Flux Isotope Reactor, Department of Energy Office of Science User Facilities operated by Oak Ridge National Laboratory. The development of the Larmor diffraction technique was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Early Career Research Program Award (No. KC0402010), under Contract No. DE-AC05-00OR22725. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. This research used resources from the Advanced Photon Source, a U.S. Department of Energy Office of Science User Facility operated for the Department of Energy Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

Funders	Funder number
National Science Foundation	DMR 2211327
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-AC05-00OR22725, KC0402010
Argonne National Laboratory	DE-AC02-06CH11357
Oak Ridge National Laboratory
Materials Research Science and Engineering Center, Harvard University	DMR 2011839

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Krysko, E., Min, L., Wang, Y., Zhang, N., Barber, J. P., Niculescu, G. E., Wright, J. T., Li, F., Burrage, K., Matsuda, M., Robinson, R. A., Zhang, Q., Katzbaer, R., Schaak, R., Terrones, M., Rost, C. M., & Mao, Z. (2023). Studies on the structure and the magnetic properties of high-entropy spinel oxide (MgMnFeCoNi)Al₂O₄. APL Materials, 11(10), Article 101123. https://doi.org/10.1063/5.0161401

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title = "Studies on the structure and the magnetic properties of high-entropy spinel oxide (MgMnFeCoNi)Al2O4",

abstract = "The study of high-entropy materials has attracted enormous interest since they could show new functional properties that are not observed in their related parent phases. Here, we report single crystal growth, structure, thermal transport, and magnetic property studies on a novel high-entropy oxide with the spinel structure (MgMnFeCoNi)Al2O4. We have successfully grown high-quality single crystals of this high-entropy oxide using the optical floating zone growth technique for the first time. The sample was confirmed to be a phase pure high-entropy oxide using x-ray diffraction and energy-dispersive spectroscopy. Through magnetization measurements, we found (MgMnFeCoNi)Al2O4 exhibits a cluster spin glass state, though the parent phases show either antiferromagnetic ordering or spin glass states. Furthermore, we also found that (MgMnFeCoNi)Al2O4 has much greater thermal expansion than its CoAl2O4 parent compound using high resolution neutron Larmor diffraction. We further investigated the structure of this high-entropy material via Raman spectroscopy and extended x-ray absorption fine structure spectroscopy (EXAFS) measurements. From Raman spectroscopy measurements, we observed (MgMnFeCoNi)Al2O4 to display a combination of the active Raman modes in its parent compounds with the modes shifted and significantly broadened. This result, together with the varying bond lengths probed by EXAFS, reveals severe local lattice distortions in this high-entropy phase. Additionally, we found a substantial decrease in thermal conductivity and suppression of the low temperature thermal conductivity peak in (MgMnFeCoNi)Al2O4, consistent with the increased lattice defects and strain. These findings advance the understanding of the dependence of thermal expansion and transport on the lattice distortions in high-entropy materials.",

author = "Evan Krysko and Lujin Min and Yu Wang and Na Zhang and Barber, {John P.} and Niculescu, {Gabriela E.} and Wright, {Joshua T.} and Fankang Li and Kaleb Burrage and Masaaki Matsuda and Robinson, {Robert A.} and Qiang Zhang and Rowan Katzbaer and Raymond Schaak and Mauricio Terrones and Rost, {Christina M.} and Zhiqiang Mao",

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AU - Krysko, Evan

AU - Min, Lujin

AU - Wang, Yu

AU - Zhang, Na

AU - Barber, John P.

AU - Niculescu, Gabriela E.

AU - Wright, Joshua T.

AU - Li, Fankang

AU - Burrage, Kaleb

AU - Matsuda, Masaaki

AU - Robinson, Robert A.

AU - Zhang, Qiang

AU - Katzbaer, Rowan

AU - Schaak, Raymond

AU - Terrones, Mauricio

AU - Rost, Christina M.

AU - Mao, Zhiqiang

PY - 2023/10/1

Y1 - 2023/10/1

N2 - The study of high-entropy materials has attracted enormous interest since they could show new functional properties that are not observed in their related parent phases. Here, we report single crystal growth, structure, thermal transport, and magnetic property studies on a novel high-entropy oxide with the spinel structure (MgMnFeCoNi)Al2O4. We have successfully grown high-quality single crystals of this high-entropy oxide using the optical floating zone growth technique for the first time. The sample was confirmed to be a phase pure high-entropy oxide using x-ray diffraction and energy-dispersive spectroscopy. Through magnetization measurements, we found (MgMnFeCoNi)Al2O4 exhibits a cluster spin glass state, though the parent phases show either antiferromagnetic ordering or spin glass states. Furthermore, we also found that (MgMnFeCoNi)Al2O4 has much greater thermal expansion than its CoAl2O4 parent compound using high resolution neutron Larmor diffraction. We further investigated the structure of this high-entropy material via Raman spectroscopy and extended x-ray absorption fine structure spectroscopy (EXAFS) measurements. From Raman spectroscopy measurements, we observed (MgMnFeCoNi)Al2O4 to display a combination of the active Raman modes in its parent compounds with the modes shifted and significantly broadened. This result, together with the varying bond lengths probed by EXAFS, reveals severe local lattice distortions in this high-entropy phase. Additionally, we found a substantial decrease in thermal conductivity and suppression of the low temperature thermal conductivity peak in (MgMnFeCoNi)Al2O4, consistent with the increased lattice defects and strain. These findings advance the understanding of the dependence of thermal expansion and transport on the lattice distortions in high-entropy materials.

AB - The study of high-entropy materials has attracted enormous interest since they could show new functional properties that are not observed in their related parent phases. Here, we report single crystal growth, structure, thermal transport, and magnetic property studies on a novel high-entropy oxide with the spinel structure (MgMnFeCoNi)Al2O4. We have successfully grown high-quality single crystals of this high-entropy oxide using the optical floating zone growth technique for the first time. The sample was confirmed to be a phase pure high-entropy oxide using x-ray diffraction and energy-dispersive spectroscopy. Through magnetization measurements, we found (MgMnFeCoNi)Al2O4 exhibits a cluster spin glass state, though the parent phases show either antiferromagnetic ordering or spin glass states. Furthermore, we also found that (MgMnFeCoNi)Al2O4 has much greater thermal expansion than its CoAl2O4 parent compound using high resolution neutron Larmor diffraction. We further investigated the structure of this high-entropy material via Raman spectroscopy and extended x-ray absorption fine structure spectroscopy (EXAFS) measurements. From Raman spectroscopy measurements, we observed (MgMnFeCoNi)Al2O4 to display a combination of the active Raman modes in its parent compounds with the modes shifted and significantly broadened. This result, together with the varying bond lengths probed by EXAFS, reveals severe local lattice distortions in this high-entropy phase. Additionally, we found a substantial decrease in thermal conductivity and suppression of the low temperature thermal conductivity peak in (MgMnFeCoNi)Al2O4, consistent with the increased lattice defects and strain. These findings advance the understanding of the dependence of thermal expansion and transport on the lattice distortions in high-entropy materials.

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ER -

Studies on the structure and the magnetic properties of high-entropy spinel oxide (MgMnFeCoNi)Al₂O₄

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