Four high-temperature ferromagnets in the Hf-Fe-Sn system

Nicholas P. Calta, Melanie C. Francisco, Christos D. Malliakas, John A. Schlueter, Mercouri G Kanatzidis

Research output: Contribution to journalArticle

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Abstract

We report the synthesis and characterization of four new ferromagnetic compounds discovered using Sn flux: Hf1.823(16)Fe5Sn3.815(14), HfFe2-xSnx, and two polymorphs of Hf1-xFe2Snx. All are closely related to HfFe2 Laves phase parent structures. HfFe2-xSnx (x ≤ 0.3-0.4) adopts the MgZn2-type (C14) crystal structure, whereas Hf1-xFe2Snx (x ≤ 0.1-0.4) adopts both the MgCu2-type (C15), and MgNi2-type (C36) structures. They crystallize in P63/mmc, Fd3¯m, and P63/mmc, respectively, with measured unit-cell parameters of a = 4.9238(7) Å and c = 7.9643(12) Å; a = 7.068(2) Å; and a = 4.9944(4) Å and c = 16.2604(15) Å, although phase width leads to a range of unit cell edge lengths. Hf1.823(16)Fe5Sn3.815(14) adopts a more complicated, incommensurately modulated structure in the superspace group Xmmm(00γ)000 with an orthorhombic subcell a = 9.7034(12) Å, b = 16.823(2) Å, and c = 8.4473(10) Å, three centering vectors of (1/2 0 0 1/2), (0 1/2 0 1/2), and (1/2 1/2 0 0), and a single-component modulation vector q = 0.2768(8)c. The structure is composed of alternating slabs of the Fe-bonded Kagomé nets observed in the HfFe2 parent structures alternated with Sn-rich Th2Zn17-type slabs, with Hf atoms primarily occurring at the interfaces between the slabs. All four compounds are ferromagnetic metals at room temperature, with Curie temperatures ranging from 467(2) to 658(2) K. Their coercive fields are remarkably low, between 2(1) and 15(2) Oe. Interestingly, in two of three cases the addition of nonmagnetic Sn atoms in place of magnetic Hf or Fe atoms in the HfFe2 structure seems to strengthen rather than weaken magnetic coupling and increase TC. Fits to electrical resistivity data for the compound suggest that electron scattering in the Laves phase polymorphs shows substantial contributions from electron-magnon and/or electron-electron scattering, while the electrical behavior of Hf1.823(16)Fe5Sn3.815(14) is dominated by electron-phonon scattering, as is the case in most metals.

Original languageEnglish
Pages (from-to)6827-6837
Number of pages11
JournalChemistry of Materials
Volume26
Issue number23
DOIs
Publication statusPublished - Dec 1 2014

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Electron scattering
Polymorphism
Atoms
Magnetic couplings
Phonon scattering
Ferromagnetic materials
Electrons
Phase structure
Curie temperature
Temperature
Crystal structure
Metals
Modulation
Fluxes

ASJC Scopus subject areas

  • Materials Chemistry
  • Chemical Engineering(all)
  • Chemistry(all)

Cite this

Calta, N. P., Francisco, M. C., Malliakas, C. D., Schlueter, J. A., & Kanatzidis, M. G. (2014). Four high-temperature ferromagnets in the Hf-Fe-Sn system. Chemistry of Materials, 26(23), 6827-6837. https://doi.org/10.1021/cm503466a

Four high-temperature ferromagnets in the Hf-Fe-Sn system. / Calta, Nicholas P.; Francisco, Melanie C.; Malliakas, Christos D.; Schlueter, John A.; Kanatzidis, Mercouri G.

In: Chemistry of Materials, Vol. 26, No. 23, 01.12.2014, p. 6827-6837.

Research output: Contribution to journalArticle

Calta, NP, Francisco, MC, Malliakas, CD, Schlueter, JA & Kanatzidis, MG 2014, 'Four high-temperature ferromagnets in the Hf-Fe-Sn system', Chemistry of Materials, vol. 26, no. 23, pp. 6827-6837. https://doi.org/10.1021/cm503466a
Calta NP, Francisco MC, Malliakas CD, Schlueter JA, Kanatzidis MG. Four high-temperature ferromagnets in the Hf-Fe-Sn system. Chemistry of Materials. 2014 Dec 1;26(23):6827-6837. https://doi.org/10.1021/cm503466a
Calta, Nicholas P. ; Francisco, Melanie C. ; Malliakas, Christos D. ; Schlueter, John A. ; Kanatzidis, Mercouri G. / Four high-temperature ferromagnets in the Hf-Fe-Sn system. In: Chemistry of Materials. 2014 ; Vol. 26, No. 23. pp. 6827-6837.
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abstract = "We report the synthesis and characterization of four new ferromagnetic compounds discovered using Sn flux: Hf1.823(16)Fe5Sn3.815(14), HfFe2-xSnx, and two polymorphs of Hf1-xFe2Snx. All are closely related to HfFe2 Laves phase parent structures. HfFe2-xSnx (x ≤ 0.3-0.4) adopts the MgZn2-type (C14) crystal structure, whereas Hf1-xFe2Snx (x ≤ 0.1-0.4) adopts both the MgCu2-type (C15), and MgNi2-type (C36) structures. They crystallize in P63/mmc, Fd3¯m, and P63/mmc, respectively, with measured unit-cell parameters of a = 4.9238(7) {\AA} and c = 7.9643(12) {\AA}; a = 7.068(2) {\AA}; and a = 4.9944(4) {\AA} and c = 16.2604(15) {\AA}, although phase width leads to a range of unit cell edge lengths. Hf1.823(16)Fe5Sn3.815(14) adopts a more complicated, incommensurately modulated structure in the superspace group Xmmm(00γ)000 with an orthorhombic subcell a = 9.7034(12) {\AA}, b = 16.823(2) {\AA}, and c = 8.4473(10) {\AA}, three centering vectors of (1/2 0 0 1/2), (0 1/2 0 1/2), and (1/2 1/2 0 0), and a single-component modulation vector q = 0.2768(8)c. The structure is composed of alternating slabs of the Fe-bonded Kagom{\'e} nets observed in the HfFe2 parent structures alternated with Sn-rich Th2Zn17-type slabs, with Hf atoms primarily occurring at the interfaces between the slabs. All four compounds are ferromagnetic metals at room temperature, with Curie temperatures ranging from 467(2) to 658(2) K. Their coercive fields are remarkably low, between 2(1) and 15(2) Oe. Interestingly, in two of three cases the addition of nonmagnetic Sn atoms in place of magnetic Hf or Fe atoms in the HfFe2 structure seems to strengthen rather than weaken magnetic coupling and increase TC. Fits to electrical resistivity data for the compound suggest that electron scattering in the Laves phase polymorphs shows substantial contributions from electron-magnon and/or electron-electron scattering, while the electrical behavior of Hf1.823(16)Fe5Sn3.815(14) is dominated by electron-phonon scattering, as is the case in most metals.",
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N2 - We report the synthesis and characterization of four new ferromagnetic compounds discovered using Sn flux: Hf1.823(16)Fe5Sn3.815(14), HfFe2-xSnx, and two polymorphs of Hf1-xFe2Snx. All are closely related to HfFe2 Laves phase parent structures. HfFe2-xSnx (x ≤ 0.3-0.4) adopts the MgZn2-type (C14) crystal structure, whereas Hf1-xFe2Snx (x ≤ 0.1-0.4) adopts both the MgCu2-type (C15), and MgNi2-type (C36) structures. They crystallize in P63/mmc, Fd3¯m, and P63/mmc, respectively, with measured unit-cell parameters of a = 4.9238(7) Å and c = 7.9643(12) Å; a = 7.068(2) Å; and a = 4.9944(4) Å and c = 16.2604(15) Å, although phase width leads to a range of unit cell edge lengths. Hf1.823(16)Fe5Sn3.815(14) adopts a more complicated, incommensurately modulated structure in the superspace group Xmmm(00γ)000 with an orthorhombic subcell a = 9.7034(12) Å, b = 16.823(2) Å, and c = 8.4473(10) Å, three centering vectors of (1/2 0 0 1/2), (0 1/2 0 1/2), and (1/2 1/2 0 0), and a single-component modulation vector q = 0.2768(8)c. The structure is composed of alternating slabs of the Fe-bonded Kagomé nets observed in the HfFe2 parent structures alternated with Sn-rich Th2Zn17-type slabs, with Hf atoms primarily occurring at the interfaces between the slabs. All four compounds are ferromagnetic metals at room temperature, with Curie temperatures ranging from 467(2) to 658(2) K. Their coercive fields are remarkably low, between 2(1) and 15(2) Oe. Interestingly, in two of three cases the addition of nonmagnetic Sn atoms in place of magnetic Hf or Fe atoms in the HfFe2 structure seems to strengthen rather than weaken magnetic coupling and increase TC. Fits to electrical resistivity data for the compound suggest that electron scattering in the Laves phase polymorphs shows substantial contributions from electron-magnon and/or electron-electron scattering, while the electrical behavior of Hf1.823(16)Fe5Sn3.815(14) is dominated by electron-phonon scattering, as is the case in most metals.

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