From phonons to the thermal properties of complex thermoelectric crystals: The case of type-I clathrates

Pailhés, S.; Giordano, Valentina M.; Turner, Shelby R; Lory, P.-F.; Candolfi, Christophe; Boissieu, M. de; Euchner, Holger

doi:10.1016/j.rinp.2023.106487

Cited by 5 publications

(2 citation statements)

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“…It was not possible to measure the thermal conductivity in our samples. However, it is interesting to give an estimate of its value in the context of recent fundamental advances in the understanding of the thermal conductivity of complex crystals, i.e., crystals with a complex crystallographic unit cell. , Indeed, it has recently been shown that complexity leads to a separation of the phonon spectrum into an optical continuum made up of a high density of modes associated with the complexity of the structures (the 3N degrees of freedom) which dominate the specific heat ( C v ∼ 3NR) and an acoustic part limited to just the three acoustic branches that dominate the lattice thermal conductivity. These two parts of the phonon spectrum are separated in energy at an energy threshold ℏω op corresponding to the energy of the lowest energy optical mode.…”

Section: Resultsmentioning

confidence: 99%

“…Ikeda et al have shown phenomenologically that the lattice thermal conductivity scales with this energy ℏω op (or corresponding temperature θ op = ℏω op / k B ) . Using the approximation of the relaxation time of the transport Boltzmann equation, Pailhès et al showed that the propagated conduction associated with acoustic branches whose dispersions are limited by ω op reads as κ false( T ≫ θ op false) = k B 6 π 2 ω op 3 v s 2 l with v s being the average sound velocity and l being the average mean free path.…”

Section: Resultsmentioning

confidence: 99%

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Stability and Physical Properties of Metastable Ba–Si Clathrates

Viennois,

Debord,

Moll

et al. 2024

Inorg. Chem.

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In the present study, we have investigated the stability of different Ba−Si clathrates with pressure and temperature using DFT calculations and studied the stability of type I Ba 8 Si 46 and type IX Ba 24 Si 100 clathrates using high pressure� high temperature synthesis technique, calorimetry, and diffraction experiments. When increasing pressure, the type I Ba 8 Si 46 clathrate and BaSi 6 become more stable. In good qualitative agreement with experiments, the type IX Ba 24 Si 100 clathrate becomes stable at a pressure of 1−2 GPa thanks to the pressure and thermal effect of both electronic and vibrational contributions. One can notice that the presence of Ba in the cages of type IX clathrate increases significantly the stability and the mechanical properties of type IX clathrate. We have determined the P−T existence domain of type IX Ba 24 Si 100 clathrate from ex situ experiments, which was confirmed by in situ synchrotron X-ray experiments. At room pressure and under an oxidizing atmosphere, the type I Ba 8 Si 46 and the type IX Ba 24 Si 100 clathrates are stable up to about 560 °C and up to about 600 °C, respectively. The thermoelectric properties of type IX Ba 24 Si 100 are also reported.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Stability and Physical Properties of Metastable Ba–Si Clathrates

Viennois,

Debord,

Moll

et al. 2024

Inorg. Chem.

Self Cite

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Influence of synthesis method and processing on the thermoelectric properties of CoSb3 skutterudites

Kumar,

Swetha,

Sahana

et al. 2024

J Mater Sci: Mater Electron

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Influence of Cationic Ordering on the Lattice Dynamics of Monoclinic Cu₅Sn₂S₇ and Cubic Cu₅Sn₂S_6.65Cl_0.35 Sulfides

Candolfi,

Le Gars,

Guélou

et al. 2024

J. Phys. Chem. C

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Cu2SnS3 is the parent compound of a series of phases in the Cu2+x Sn1–x S3 section (0 ≤ x ≤ 0.15) of the ternary Cu–Sn–S phase diagram, the crystal structure of which can be controlled by varying the synthesis process and/or through a fine-tuning of the chemical composition. Despite being structurally close to the sphalerite structure, the thermal transport of these compounds is strongly dependent on the exact lattice symmetry and degree of atomic disorder. Here, we investigate the lattice dynamics of the monoclinic ordered Cu5Sn2S7 (space group C2) and cubic disordered Cu5Sn2S6.65Cl0.35 (space group F4̅3m) compounds by temperature-dependent powder inelastic neutron scattering (INS). In both cases, the INS spectra feature low-energy optical modes mostly weighed by the thermal motion of Cu atoms. The response of the INS spectra of Cu5Sn2S6.65Cl0.35 to temperature variations is indicative of quasi-harmonic behavior. Combined with analyses of the low-temperature specific heat, these findings show that the significant lowering of the lattice thermal conductivity in cubic Cu5Sn2S6.65Cl0.35 is due to a reduced phonon mean free path tied to the increased level of disorder in the unit cell. These results highlight how the stabilization of highly symmetric, yet strongly disordered crystal structures akin to those observed in high-entropy alloys, can lead to a drastic reduction in the heat transport, offering an effective approach to design high-performance thermoelectric sulfides.

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From phonons to the thermal properties of complex thermoelectric crystals: The case of type-I clathrates

Cited by 5 publications

References 58 publications

Stability and Physical Properties of Metastable Ba–Si Clathrates

Stability and Physical Properties of Metastable Ba–Si Clathrates

Influence of synthesis method and processing on the thermoelectric properties of CoSb3 skutterudites

Influence of Cationic Ordering on the Lattice Dynamics of Monoclinic Cu₅Sn₂S₇ and Cubic Cu₅Sn₂S_6.65Cl_0.35 Sulfides

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From phonons to the thermal properties of complex thermoelectric crystals: The case of type-I clathrates

Cited by 5 publications

References 58 publications

Stability and Physical Properties of Metastable Ba–Si Clathrates

Stability and Physical Properties of Metastable Ba–Si Clathrates

Influence of synthesis method and processing on the thermoelectric properties of CoSb3 skutterudites

Influence of Cationic Ordering on the Lattice Dynamics of Monoclinic Cu5Sn2S7 and Cubic Cu5Sn2S6.65Cl0.35 Sulfides

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Product

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Influence of Cationic Ordering on the Lattice Dynamics of Monoclinic Cu₅Sn₂S₇ and Cubic Cu₅Sn₂S_6.65Cl_0.35 Sulfides