Nd ordering, cluster formation, and the origin of negative magnetization in NdMn0.8Fe0.2O3+δ

D. M. Pajerowski; C. A. Escanhoela; D. Haskel; T. R. Prisk; M. D. Frontzek; D. Phelan; M. Mihalik

doi:10.1016/j.jmmm.2019.165968

Nd ordering, cluster formation, and the origin of negative magnetization in NdMn_0.8Fe_0.2O_3+δ

D. M. Pajerowski, C. A. Escanhoela, D. Haskel, T. R. Prisk, M. D. Frontzek, D. Phelan, M. Mihalik

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Abstract

The orthorhombic pseudo-perovskite series NdMn_1-xFe_xO_3+δ has negative magnetization, i.e. magnetization directed opposite to an applied field under certain conditions, for x = 0.2 and x = 0.25. We have investigated the microscopic origin of this phenomenon for x = 0.2 by using elastic and inelastic scattering techniques including neutron backscattering, X-ray magnetic circular dichroism at the Mn K and Nd L₂ edges, neutron powder diffraction, and powder inelastic neutron scattering. We find that Nd³⁺ ions possess zero field ordered moments of 1.6 μ_B per ion at 1.5 K oriented parallel to the Mn moments. Based upon the neutron diffraction, there is a freezing of magnetic clusters before the long-range order sets in. The Nd crystal field levels shift with temperature due to a molecular field that is 1.1 meV at 1.5 K. These findings are consistent with a magnetic domain/cluster model for the negative magnetization in NdMn_0.8Fe_0.2O_3+δ.

Original language	English
Article number	165968
Journal	Journal of Magnetism and Magnetic Materials
Volume	497
DOIs	https://doi.org/10.1016/j.jmmm.2019.165968
State	Published - Mar 1 2020

Funding

This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). The work at Oak Ridge National Laboratories’ High Flux Isotope Reactor was supported by the United States Department of Energy (US-DOE), Office of Science – Basic Energy Science (BES), Scientific User Facilities Division. Access to HFBS was provided by the Center for High Resolution Neutron Scattering, a partnership between the National Institute of Standards and Technology and the National Science Foundation under Agreement No. DMR-1508249. Work at Argonne is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC-02-06CH11357. C.A.E. Jr. was supported by FAPESP (SP-Brazil) under Contract No. 2016/24137-3 . Sample preparation at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division. Work at IEP SAS is supported by the project VEGA 2/0137/19. The work at Oak Ridge National Laboratories? High Flux Isotope Reactor was supported by the United States Department of Energy (US-DOE), Office of Science ? Basic Energy Science (BES), Scientific User Facilities Division. Access to HFBS was provided by the Center for High Resolution Neutron Scattering, a partnership between the National Institute of Standards and Technology and the National Science Foundation under Agreement No. DMR-1508249. Work at Argonne is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC-02-06CH11357. C.A.E. Jr. was supported by FAPESP (SP-Brazil) under Contract No. 2016/24137-3. Sample preparation at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division. Work at IEP SAS is supported by the project VEGA 2/0137/19.

Funders	Funder number
Basic Energy Science
Materials Science and Engineering Division
Office of Basic Energy Sciences
Office of Science ?
Office of Science – Basic Energy Science
SP-Brazil	2016/24137-3
United States Department of Energy
National Science Foundation	DMR-1508249
U.S. Department of Energy
National Institute of Standards and Technology
Office of Science
Basic Energy Sciences	DE-AC-02-06CH11357
Argonne National Laboratory
Oak Ridge National Laboratory
Division of Materials Sciences and Engineering
Fundação de Amparo à Pesquisa do Estado de São Paulo
Vedecká Grantová Agentúra MŠVVaŠ SR a SAV	2/0137/19

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title = "Nd ordering, cluster formation, and the origin of negative magnetization in NdMn0.8Fe0.2O3+δ ",

abstract = "The orthorhombic pseudo-perovskite series NdMn1-xFexO3+δ has negative magnetization, i.e. magnetization directed opposite to an applied field under certain conditions, for x = 0.2 and x = 0.25. We have investigated the microscopic origin of this phenomenon for x = 0.2 by using elastic and inelastic scattering techniques including neutron backscattering, X-ray magnetic circular dichroism at the Mn K and Nd L2 edges, neutron powder diffraction, and powder inelastic neutron scattering. We find that Nd3+ ions possess zero field ordered moments of 1.6 μB per ion at 1.5 K oriented parallel to the Mn moments. Based upon the neutron diffraction, there is a freezing of magnetic clusters before the long-range order sets in. The Nd crystal field levels shift with temperature due to a molecular field that is 1.1 meV at 1.5 K. These findings are consistent with a magnetic domain/cluster model for the negative magnetization in NdMn0.8Fe0.2O3+δ.",

author = "Pajerowski, {D. M.} and Escanhoela, {C. A.} and D. Haskel and Prisk, {T. R.} and Frontzek, {M. D.} and D. Phelan and M. Mihalik",

note = "Publisher Copyright: {\textcopyright} 2019 Elsevier B.V.",

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doi = "10.1016/j.jmmm.2019.165968",

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T1 - Nd ordering, cluster formation, and the origin of negative magnetization in NdMn0.8Fe0.2O3+δ

AU - Pajerowski, D. M.

AU - Escanhoela, C. A.

AU - Haskel, D.

AU - Prisk, T. R.

AU - Frontzek, M. D.

AU - Phelan, D.

AU - Mihalik, M.

PY - 2020/3/1

Y1 - 2020/3/1

N2 - The orthorhombic pseudo-perovskite series NdMn1-xFexO3+δ has negative magnetization, i.e. magnetization directed opposite to an applied field under certain conditions, for x = 0.2 and x = 0.25. We have investigated the microscopic origin of this phenomenon for x = 0.2 by using elastic and inelastic scattering techniques including neutron backscattering, X-ray magnetic circular dichroism at the Mn K and Nd L2 edges, neutron powder diffraction, and powder inelastic neutron scattering. We find that Nd3+ ions possess zero field ordered moments of 1.6 μB per ion at 1.5 K oriented parallel to the Mn moments. Based upon the neutron diffraction, there is a freezing of magnetic clusters before the long-range order sets in. The Nd crystal field levels shift with temperature due to a molecular field that is 1.1 meV at 1.5 K. These findings are consistent with a magnetic domain/cluster model for the negative magnetization in NdMn0.8Fe0.2O3+δ.

AB - The orthorhombic pseudo-perovskite series NdMn1-xFexO3+δ has negative magnetization, i.e. magnetization directed opposite to an applied field under certain conditions, for x = 0.2 and x = 0.25. We have investigated the microscopic origin of this phenomenon for x = 0.2 by using elastic and inelastic scattering techniques including neutron backscattering, X-ray magnetic circular dichroism at the Mn K and Nd L2 edges, neutron powder diffraction, and powder inelastic neutron scattering. We find that Nd3+ ions possess zero field ordered moments of 1.6 μB per ion at 1.5 K oriented parallel to the Mn moments. Based upon the neutron diffraction, there is a freezing of magnetic clusters before the long-range order sets in. The Nd crystal field levels shift with temperature due to a molecular field that is 1.1 meV at 1.5 K. These findings are consistent with a magnetic domain/cluster model for the negative magnetization in NdMn0.8Fe0.2O3+δ.

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VL - 497

JO - Journal of Magnetism and Magnetic Materials

JF - Journal of Magnetism and Magnetic Materials

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ER -

Nd ordering, cluster formation, and the origin of negative magnetization in NdMn_0.8Fe_0.2O_3+δ

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