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Breakdown of phonon glass paradigm in La- and Ce-filled Fe4Sb12 skutterudites

Nature Materials volume 7, pages 805–810 (2008)Cite this article

Abstract

The material class of skutterudites is believed to have strong potential for thermoelectric application due to the very low thermal conductivity of the filled structures. It is generally assumed that the atoms filling the skutterudite cages act as ‘rattlers’ and essentially induce a disordered lattice dynamics referred to as ‘phonon glass’. Here, we present neutron spectroscopy experiments and ab initio computational work on phonons in LaFe4Sb12 and CeFe4Sb12. Our results give unequivocal evidence of essentially temperature-independent lattice dynamics with well-defined phase relations between guest and host dynamics, indicative of a quasi-harmonic coupling between the guests and the host lattice. These conclusions are in disagreement with the ‘phonon glass’ paradigm based on individual ‘rattling’ of the guest atoms. These findings should have an essential impact on the design and improvement of thermoelectric materials and on the development of microscopic models needed for these efforts.

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Figure 1: Schematic presentation of the conceptual ‘rattling’ mode framework referred to in this article.
Figure 2: Measured powder-averaged response of a LaFe4Sb12 sample.
Figure 3: Calculated powder-averaged response of a LaFe4Sb12 sample.
Figure 4: Momentum-averaged spectral density of LaFe4Sb12 and CeFe4Sb12.
Figure 5: Energy transfer dependence of the experimental response compared with PALD.
Figure 6: Momentum transfer dependence of the experimental response compared with PALD.

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Authors and Affiliations

  1. Institut Laue Langevin, 6 Rue Jules Horowitz, B.P. 156, 38042 Grenoble, Cedex 9, France

    Michael Marek Koza, Mark Robert Johnson & Hannu Mutka

  2. DPMC, Universite de Geneve, 24 quai Ernest Ansermet, CH-1211 Geneva, Switzerland

    Romain Viennois

  3. LPMC, Universite de Montpellier II, pl. Eugene Bataillon, 34095 Montpellier, France

    Luc Girard & Didier Ravot

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  1. Michael Marek Koza
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Correspondence to Michael Marek Koza.

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Koza, M., Johnson, M., Viennois, R. et al. Breakdown of phonon glass paradigm in La- and Ce-filled Fe4Sb12 skutterudites. Nature Mater 7, 805–810 (2008). https://doi.org/10.1038/nmat2260

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