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See detailLattice dynamics in thermoelectric Zintl phases
Möchel, Anne ULg

Doctoral thesis (2011)

A brief introduction to the thermoelectric effects, the studied materials, and the experimen- tal methods is given in the first chapter. The introduction is not intended to be exhaustive, but only to ... [more ▼]

A brief introduction to the thermoelectric effects, the studied materials, and the experimen- tal methods is given in the first chapter. The introduction is not intended to be exhaustive, but only to summarize important basic information for the reader. The introduction is followed by four chapters dedicated to detailed experimental studies of the lattice dynamics in selected thermoelectric Zintl phases. First, the lattice dynamics in the unfilled and filled skutterudites FeSb3 , CoSb3 , and YbFe4 Sb12 were studied by nuclear inelastic scattering, inelastic neutron scattering, and several macroscopic methods. These studies reveal that FeSb3 exhibits softer Sb bonds than CoSb3 , that the density of phonon states is shifted towards lower energies and the velocity of sound is lower in FeSb3 as compared to CoSb3 . It appears thus that the soft [Fe4 Sb12 ] framework dynamics might play an important role in the thermoelectric properties of filled skutterudites. The observed anomalous temperature dependence of the elastic constants and the rearrangement of the spectral weight of the Yb phonon states in YbFe4 Sb12 can be explained by a change of the Yb valence state with the temperature. Second, the lattice dynamics in the Sr8 Ga16 Ge30 clathrate was investigated by inelastic neutron scattering measurements on a single crystal. We found that several mechanisms contribute to the low thermal conductivity in this system and that the reduction of the heat capacity contribution to the thermal conductivity plays a significant role to the low thermal conductivity, besides the reduction in the phonon lifetime and the phonon group velocity that is related to the guest atom. Third, the lattice dynamics of the Zintl phase Yb14 MnSb11 was studied by inelastic neu- tron scattering and nuclear inelastic scattering measurements. All phonon modes of these complex crystal systems are in a narrow energy range below ∼25 meV and the Debye tem- perature, the velocity of sound and the mean force constants are small compared to those of other thermoelectric materials such as Zn4 Sb3 . By comparing the lattice dynamics in Yb14 MnSb11 and Zn4 Sb3 different mechanisms which lead to the low thermal conductivity in Zintl phases have been identified. Between 300 and 1200 K no softening of the velocity of sound in Yb14 MnSb11 was observed by temperature dependent inelastic neutron scattering measurements, which is in line with its large melting temperature. [less ▲]

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See detailA study of low-energy guest phonon modes in clathrate-II NaxSi136 (x = 3, 23, and 24)
Beekman, M.; Hermann, Raphaël ULg; Möchel, Anne ULg et al

in Journal of Physics : Condensed Matter (2010)

Single-crystal x-ray diffraction from clathrate-II NaxSi136 (x = 24) prepared by a new technique reveals the exceptionally large Na@Si-28 atomic displacement parameter (U-eq) is strongly temperature ... [more ▼]

Single-crystal x-ray diffraction from clathrate-II NaxSi136 (x = 24) prepared by a new technique reveals the exceptionally large Na@Si-28 atomic displacement parameter (U-eq) is strongly temperature dependent, and can be attributed to low-energy rattling modes associated with the Na guest. Inelastic neutron scattering (INS) spectra collected from NaxSi136 powder specimens (x = 3, 23) confirm the presence of low-energy guest-derived phonon modes for Na@Si-28 and Na@Si-20. The lower energy Na@Si-28 rattler mode falls in the frequency range of the silicon host acoustic phonons, indicating the possibility for interaction with these phonons. The presence of these low-energy modes combined with the ability to controllably vary the guest content presents a unique opportunity for exploring the influence of guest-framework interactions on the lattice dynamics in intermetallic clathrates. [less ▲]

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See detailNuclear forward and inelastic spectroscopy on 125Te and Sb2 125Te3 2
Wille, H.-C.; Hermann, Raphaël ULg; Sergueev, I. et al

in Europhysics Letters [=EPL] (2010)

We report on the observation of nuclear forward and nuclear inelastic scattering of synchrotron radiation by Te-125 and the application of both spectroscopic methods to tellurium compounds by using a high ... [more ▼]

We report on the observation of nuclear forward and nuclear inelastic scattering of synchrotron radiation by Te-125 and the application of both spectroscopic methods to tellurium compounds by using a high-resolution backscattering sapphire monochromator in combination with fast detection electronics. The lifetime of the nuclear resonance and the energy of the transition were determined to be 2.131(12) ns and 35493.12(30) eV, respectively. As applications, the nuclear inelastic spectrum in Sb2Te3 and the nuclear forward scattering by Te metal were measured. These measurements open the field of nuclear resonance spectroscopy on tellurium compounds such as thermoelectric and superconducting materials. [less ▲]

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