Magnetic properties of Fe 2GeMo 3N; An experimental and computational study

Peter D. Battle, Lev A. Sviridov, Russell J. Woolley, Fernande Grandjean, Gary J. Long, C. Richard A. Catlow, Alexey A. Sokol, Aron Walsh, Scott M. Woodley

Research output: Contribution to journalArticle

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Abstract

A polycrystalline sample of Fe 2GeMo 3N has been synthesized by the reductive nitridation of a mixture of binary oxides in a flow of 10% dihydrogen in dinitrogen. The reaction product has been studied by magnetometry, neutron diffraction and Mössbauer spectroscopy over the temperature range 1.8 ≤ T/K ≤ 700. The electronic structure and magnetic coupling have been modelled by Density Functional Theory (DFT) and Monte Carlo methods. Fe 2GeMo 3N adopts the cubic η-carbide structure with a = 11.1630(1) Å at 300 K. The electrical resistivity was found to be ∼0.9 mΩ cm over the temperature range 80 ≤ T/K ≤ 300. On cooling below 455 K the compound undergoes a transition from a paramagnetic to an antiferromagnetic state. The magnetic unit cell contains an antiferromagnetic arrangement of eight ferromagnetic Fe 4 tetrahedra; the ordered atomic magnetic moments, 1.90(4) μ B per Fe atom at 1.8 K, align along a <111> direction. DFT predicts an ordered moment of 1.831 μ B per Fe. A random phase approximation to the DFT parameterised Heisenberg model yields a Néel temperature of 549 K, whereas the value of 431 K is obtained in the classical limit for spin. Monte Carlo calculations confirm that the experimentally determined magnetic structure is the lowest-energy antiferromagnetic structure, but with a lower Néel temperature of 412 K. These results emphasise the potential of these computational methods in the search for new magnetic materials.

Original languageEnglish
Pages (from-to)15606-15613
Number of pages8
JournalJournal of Materials Chemistry
Volume22
Issue number31
DOIs
Publication statusPublished - 2012 Aug 21

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Magnetic properties
Density functional theory
Magnetic couplings
Temperature
Nitridation
Magnetic structure
Magnetic materials
Neutron diffraction
Computational methods
Magnetic moments
Reaction products
Oxides
Electronic structure
Carbides
Monte Carlo methods
Spectroscopy
Cooling
Atoms

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Materials Chemistry

Cite this

Battle, P. D., Sviridov, L. A., Woolley, R. J., Grandjean, F., Long, G. J., Catlow, C. R. A., ... Woodley, S. M. (2012). Magnetic properties of Fe 2GeMo 3N; An experimental and computational study. Journal of Materials Chemistry, 22(31), 15606-15613. https://doi.org/10.1039/c2jm32574h
Battle, Peter D. ; Sviridov, Lev A. ; Woolley, Russell J. ; Grandjean, Fernande ; Long, Gary J. ; Catlow, C. Richard A. ; Sokol, Alexey A. ; Walsh, Aron ; Woodley, Scott M. / Magnetic properties of Fe 2GeMo 3N; An experimental and computational study. In: Journal of Materials Chemistry. 2012 ; Vol. 22, No. 31. pp. 15606-15613.
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Battle, PD, Sviridov, LA, Woolley, RJ, Grandjean, F, Long, GJ, Catlow, CRA, Sokol, AA, Walsh, A & Woodley, SM 2012, 'Magnetic properties of Fe 2GeMo 3N; An experimental and computational study', Journal of Materials Chemistry, vol. 22, no. 31, pp. 15606-15613. https://doi.org/10.1039/c2jm32574h

Magnetic properties of Fe 2GeMo 3N; An experimental and computational study. / Battle, Peter D.; Sviridov, Lev A.; Woolley, Russell J.; Grandjean, Fernande; Long, Gary J.; Catlow, C. Richard A.; Sokol, Alexey A.; Walsh, Aron; Woodley, Scott M.

In: Journal of Materials Chemistry, Vol. 22, No. 31, 21.08.2012, p. 15606-15613.

Research output: Contribution to journalArticle

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T1 - Magnetic properties of Fe 2GeMo 3N; An experimental and computational study

AU - Battle, Peter D.

AU - Sviridov, Lev A.

AU - Woolley, Russell J.

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AU - Long, Gary J.

AU - Catlow, C. Richard A.

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AU - Walsh, Aron

AU - Woodley, Scott M.

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N2 - A polycrystalline sample of Fe 2GeMo 3N has been synthesized by the reductive nitridation of a mixture of binary oxides in a flow of 10% dihydrogen in dinitrogen. The reaction product has been studied by magnetometry, neutron diffraction and Mössbauer spectroscopy over the temperature range 1.8 ≤ T/K ≤ 700. The electronic structure and magnetic coupling have been modelled by Density Functional Theory (DFT) and Monte Carlo methods. Fe 2GeMo 3N adopts the cubic η-carbide structure with a = 11.1630(1) Å at 300 K. The electrical resistivity was found to be ∼0.9 mΩ cm over the temperature range 80 ≤ T/K ≤ 300. On cooling below 455 K the compound undergoes a transition from a paramagnetic to an antiferromagnetic state. The magnetic unit cell contains an antiferromagnetic arrangement of eight ferromagnetic Fe 4 tetrahedra; the ordered atomic magnetic moments, 1.90(4) μ B per Fe atom at 1.8 K, align along a <111> direction. DFT predicts an ordered moment of 1.831 μ B per Fe. A random phase approximation to the DFT parameterised Heisenberg model yields a Néel temperature of 549 K, whereas the value of 431 K is obtained in the classical limit for spin. Monte Carlo calculations confirm that the experimentally determined magnetic structure is the lowest-energy antiferromagnetic structure, but with a lower Néel temperature of 412 K. These results emphasise the potential of these computational methods in the search for new magnetic materials.

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Battle PD, Sviridov LA, Woolley RJ, Grandjean F, Long GJ, Catlow CRA et al. Magnetic properties of Fe 2GeMo 3N; An experimental and computational study. Journal of Materials Chemistry. 2012 Aug 21;22(31):15606-15613. https://doi.org/10.1039/c2jm32574h