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Title: Enhancing Magnetic Functionality with Scandium: Breaking Stereotypes in the Design of Rare Earth Materials

Abstract

Replacement of strongly magnetic gadolinium with weakly magnetic scandium unexpectedly enhances ferromagnetic interactions in (Gd1–xScx)5Ge4. Based upon this counterintuitive experimental finding we demonstrate the unique role 3d1 electrons of scandium atoms play in mediating magnetic interactions between the gadolinium atoms from the neighboring layers in the Sm5Ge4-type crystal lattice. Scandium substitutions at and below 20% rapidly increase the Curie temperature, TC, of the Gd5Ge4 parent, eliminate both the kinetic arrest and hysteresis, and drastically improve reversibility of the first-order magnetostructural transformation at TC. In agreement with first-principles predictions, higher than 20% Sc leads to the formation of a closely related Pu5Rh4-type structure where the first-order magnetostructural transformation is replaced by a conventional second-order ferromagnetic ordering that remains accompanied by a continuous rearrangement of the crystal lattice. In conclusion, comparison of two materials with similar structures and compositions shows that significantly stronger magnetocaloric effect occurs in the first-order material, which also shows very small hysteresis. Furthermore, we demonstrate that a behavior of a specific interatomic distance can predict anomalous physical properties in a series of alloys where compositional dependence of lattice parameters suggests a rather trivial solid solubility and uninteresting magnetism.

Authors:
ORCiD logo; ; ;
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1355454
Report Number(s):
IS-J-9303
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 9; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Mudryk, Yaroslav, Paudyal, Durga, Liu, Jing, and Pecharsky, Vitalij K. Enhancing Magnetic Functionality with Scandium: Breaking Stereotypes in the Design of Rare Earth Materials. United States: N. p., 2017. Web. doi:10.1021/acs.chemmater.7b00314.
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Mudryk, Yaroslav, Paudyal, Durga, Liu, Jing, & Pecharsky, Vitalij K. Enhancing Magnetic Functionality with Scandium: Breaking Stereotypes in the Design of Rare Earth Materials. United States. https://doi.org/10.1021/acs.chemmater.7b00314
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Mudryk, Yaroslav, Paudyal, Durga, Liu, Jing, and Pecharsky, Vitalij K. Tue . "Enhancing Magnetic Functionality with Scandium: Breaking Stereotypes in the Design of Rare Earth Materials". United States. https://doi.org/10.1021/acs.chemmater.7b00314. https://www.osti.gov/servlets/purl/1355454.
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@article{osti_1355454,
title = {Enhancing Magnetic Functionality with Scandium: Breaking Stereotypes in the Design of Rare Earth Materials},
author = {Mudryk, Yaroslav and Paudyal, Durga and Liu, Jing and Pecharsky, Vitalij K.},
abstractNote = {Replacement of strongly magnetic gadolinium with weakly magnetic scandium unexpectedly enhances ferromagnetic interactions in (Gd1–xScx)5Ge4. Based upon this counterintuitive experimental finding we demonstrate the unique role 3d1 electrons of scandium atoms play in mediating magnetic interactions between the gadolinium atoms from the neighboring layers in the Sm5Ge4-type crystal lattice. Scandium substitutions at and below 20% rapidly increase the Curie temperature, TC, of the Gd5Ge4 parent, eliminate both the kinetic arrest and hysteresis, and drastically improve reversibility of the first-order magnetostructural transformation at TC. In agreement with first-principles predictions, higher than 20% Sc leads to the formation of a closely related Pu5Rh4-type structure where the first-order magnetostructural transformation is replaced by a conventional second-order ferromagnetic ordering that remains accompanied by a continuous rearrangement of the crystal lattice. In conclusion, comparison of two materials with similar structures and compositions shows that significantly stronger magnetocaloric effect occurs in the first-order material, which also shows very small hysteresis. Furthermore, we demonstrate that a behavior of a specific interatomic distance can predict anomalous physical properties in a series of alloys where compositional dependence of lattice parameters suggests a rather trivial solid solubility and uninteresting magnetism.},
doi = {10.1021/acs.chemmater.7b00314},
journal = {Chemistry of Materials},
number = 9,
volume = 29,
place = {United States},
year = {Tue Apr 11 00:00:00 EDT 2017},
month = {Tue Apr 11 00:00:00 EDT 2017}
}
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https://doi.org/10.1021/acs.chemmater.7b00314
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Works referenced in this record:

Taming the First-Order Transition in Giant Magnetocaloric Materials
journal, February 2014

  • Guillou, François; Porcari, Giacomo; Yibole, Hargen
  • Advanced Materials, Vol. 26, Issue 17
  • DOI: 10.1002/adma.201304788

Magnetic properties of high purity scandium and the effect of impurities on these properties
journal, June 1973

  • Spedding, F. H.; Croat, J. J.
  • The Journal of Chemical Physics, Vol. 58, Issue 12
  • DOI: 10.1063/1.1679173

The properties and application of scandium-reinforced aluminum
journal, February 2003

A new symmetric solid-oxide fuel cell with La0.8Sr0.2Sc0.2Mn0.8O3-δ perovskite oxide as both the anode and cathode
journal, February 2009

High magnetic transition temperatures in RScT (R=Pr, Nd and Sm; T=Si and Ge) compounds: multiple spin reorientations in PrScGe
journal, February 2004

Single crystal study of the high-Curie-temperature ferromagnet Gd1.02Sc0.98Ge and of Gd2.38Sc2.62Ge3
journal, February 2002

Structure, magnetism, and thermodynamics of the novel rare earth-based R5T4 intermetallics
journal, January 2007

Giant Magnetocaloric Effect in Gd5(Si2Ge2)
journal, June 1997

Tunable magnetic regenerator alloys with a giant magnetocaloric effect for magnetic refrigeration from ∼20 to ∼290 K
journal, June 1997

  • Pecharsky, V. K.; Gschneidner, K. A.
  • Applied Physics Letters, Vol. 70, Issue 24
  • DOI: 10.1063/1.119206

Recent developments in magnetocaloric materials
journal, May 2005

  • Gschneidner, K. A.; Pecharsky, V. K.; Tsokol, A. O.
  • Reports on Progress in Physics, Vol. 68, Issue 6, p. 1479-1539
  • DOI: 10.1088/0034-4885/68/6/R04

Magnetic-field-induced structural phase transition in Gd 5 ( S i 1.8 Ge 2.2 )
journal, December 1998

Magnetoelastic behaviour of Gd 5 Ge 4
journal, March 2003

Giant magnetoresistance near the magnetostructural transition in Gd5(Si1.8Ge2.2)
journal, December 1998

  • Morellon, L.; Stankiewicz, J.; Garcı́a-Landa, B.
  • Applied Physics Letters, Vol. 73, Issue 23
  • DOI: 10.1063/1.122797

Electrical resistivity and magnetoresistance of single-crystal Tb 5 Si 2.2 Ge 1.8
journal, November 2009

Spontaneous generation of voltage in Gd 5 ( Si x Ge 4 − x ) during a first-order phase transition induced by temperature or magnetic field
journal, April 2001

Evidence of a magnetic glass state in the magnetocaloric material Gd 5 Ge 4
journal, July 2006

Field step size and temperature effects on the character of the magnetostructural transformation in a Gd 5 Ge 4 single crystal
journal, October 2007

Short-range anisotropic ferromagnetic correlations in the paramagnetic and antiferromagnetic phases of Gd 5 Ge 4
journal, September 2006

Griffiths-like phase of magnetocaloric R 5 ( Si x Ge 1 − x ) 4 ( R = Gd , Tb, Dy, and Ho)
journal, November 2010

Gd5(SixGe1-x)4: An Extremum Material
journal, May 2001

“Nanoscale Zippers” in the Crystalline Solid. Structural Variations in the Giant Magnetocaloric Material Gd 5 Si 1.5 Ge 2.5
journal, April 2003

  • Choe, Wonyoung; Miller, Gordon J.; Meyers, John
  • Chemistry of Materials, Vol. 15, Issue 7
  • DOI: 10.1021/cm020928l

Magnetic structure of Gd 5 Ge 4
journal, June 2005

Role of Ge in Bridging Ferromagnetism in the Giant Magnetocaloric Gd 5 ( Ge 1 − x Si x ) 4 Alloys
journal, June 2007

Controlling Magnetism of a Complex Metallic System Using Atomic Individualism
journal, August 2010

Structural and magnetic properties of the ternary compounds Gd2Sc3X4 with X=Si and Ge
journal, May 2011

X-ray powder diffractometer for in situ structural studies in magnetic fields from 0 to 35 kOe between 2.2 and 315 K
journal, April 2004

  • Holm, Aaron Patrick; Pecharsky, Vitalij K.; Gschneidner, Karl A.
  • Review of Scientific Instruments, Vol. 75, Issue 4
  • DOI: 10.1063/1.1667253

First-principles calculations of the electronic structure and spectra of strongly correlated systems: the LDA + U method
journal, January 1997

  • Anisimov, Vladimir I.; Aryasetiawan, F.; Lichtenstein, A. I.
  • Journal of Physics: Condensed Matter, Vol. 9, Issue 4, p. 767-808
  • DOI: 10.1088/0953-8984/9/4/002

Explicit, First-Principles Tight-Binding Theory
journal, December 1984

Origin of Magnetic Anisotropy of Gd Metal
journal, October 2003

Magnetic anisotropy in Gd, GdN, and GdFe 2 tuned by the energy of gadolinium 4 f states
journal, February 2009

Gadolinium scandium germanide, Gd 2 Sc 3 Ge 4
journal, March 2009

  • Misra, Sumohan; Miller, Gordon J.
  • Acta Crystallographica Section E Structure Reports Online, Vol. 65, Issue 4
  • DOI: 10.1107/S1600536809007211

Massive Magnetic-Field-Induced Structural Transformation in G d 5 G e 4 and the Nature of the Giant Magnetocaloric Effect
journal, November 2003

Competing crystal and magnetic structures in Gd 5 Ge 4
journal, October 2010

Influence of Y substitutions on the magnetism of Gd5Ge4
journal, May 2010

  • Paudyal, Durga; Mudryk, Y.; Pecharsky, V. K.
  • Journal of Applied Physics, Vol. 107, Issue 9
  • DOI: 10.1063/1.3349231

Pressure-induced removal of magnetostructural inhomogeneity in Ge-rich Gd 5 ( Si x Ge 1 − x ) 4 giant magnetocaloric alloys
journal, December 2008

Unusual magnetic frustration in Lu-doped Gd 5 Ge 4
journal, May 2013

  • Mudryk, Y.; Pecharsky, V. K.; Gschneidner, K. A.
  • Journal of Applied Physics, Vol. 113, Issue 17
  • DOI: 10.1063/1.4793600

Observation of a Griffiths-like Phase in the Magnetocaloric Compound Tb 5 Si 2 Ge 2
journal, April 2006

New ferromagnetic 5 : 4 compounds in the rare earth silicon and germanium systems
journal, November 1967

  • Holtzberg, F.; Gambino, R. J.; McGuire, T. R.
  • Journal of Physics and Chemistry of Solids, Vol. 28, Issue 11
  • DOI: 10.1016/0022-3697(67)90253-3
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    Works referencing / citing this record:

    Lanthanum Dilution Effects on the Giant Magnetocaloric Gd 5 Si 1.8 Ge 2.2 Compound
    journal, September 2018

    • Andrade, Vivian M.; Belo, João H.; Reis, Mario S.
    • physica status solidi (b), Vol. 255, Issue 10
    • DOI: 10.1002/pssb.201800101

    Carbon Cloth Supported Nano-Mg(OH)2 for the Enrichment and Recovery of Rare Earth Element Eu(III) From Aqueous Solution
    journal, April 2018

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