Localized vibrational modes in metallic solids

V. Keppens, D. Mandrus, B. C. Sales, B. C. Chakoumakos (), P. Dai, R. Coldea, M. B. Maple, D. A. Gajewski, E. J. Freeman and S. Bennington
Additional contact information
V. Keppens: Oak Ridge National Laboratory
D. Mandrus: Oak Ridge National Laboratory
B. C. Sales: Oak Ridge National Laboratory
B. C. Chakoumakos: Oak Ridge National Laboratory
P. Dai: Oak Ridge National Laboratory
R. Coldea: Oak Ridge National Laboratory
M. B. Maple: University of California San Diego
D. A. Gajewski: University of California San Diego
E. J. Freeman: University of California San Diego
S. Bennington: ISIS Facility, Rutherford Appleton Laboratory

Nature, 1998, vol. 395, issue 6705, 876-878

Abstract: Abstract Filled skutterudite antimonides1,2 are cubic compounds with the formula RM4Sb12, where R is a rare-earth element (such as La or Ce), and M is a transition metal (for example, Fe or Co). The rare-earth ion is weakly bound in an oversized atomic cage formed by the other atoms. Its presence has been shown to cause a dramatic reduction in the lattice component of the thermal conductivity, while having little effect on the electronic properties3,4,5 of the compound. This combination of properties makes filled skutterudites of interest as thermoelectric materials. It has been suggested4 that localized, incoherent vibrations of the rare-earth ion are responsible for the reduction in thermal conductivity, but no direct evidence for these local vibrational modes exists. Here we report the observation of local modes in La-filled skutterudites, using heat capacity, elastic constant and inelastic neutron scattering measurements. The La atoms show unusual thermodynamic behaviour, characterized by the presence of two low-energy localized modes. Our results suggest that consideration of local modes will play an important role in the design of the next generation of thermoelectric materials.

Date: 1998
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DOI: 10.1038/27625

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