Ab initio studies on the lattice thermal conductivity of silicon clathrate frameworks II and VIII

Abstract

The lattice thermal conductivities of silicon clathrate frameworks II and VIII are investigated by using ab initio lattice dynamics and iterative solution of the linearized Boltzmann transport equation(BTE) for phonons. Within the temperature range 100-350 K, the clathrate structures II and VIII were found to have lower lattice thermal conductivity values than silicon diamond structure (d-Si) by factors of 1/2 and 1/5, respectively. The main reason for the lower lattice thermal conductivity of the clathrate structure II in comparison to d-Si was found to be the harmonic phonon spectra, while in the case of the clathrate structure VIII, the difference is mainly due to the harmonic phonon spectra and partly due to shorter relaxation times of phonons. In the studied clathrate frameworks, the anharmonic effects have larger impact on the lattice thermal conductivity than the size of the unit cell. For the structure II, the predicted lattice thermal conductivity differs approximately by factor of 20 from the previous experimental results obtained for a polycrystalline sample at room temperature.

12 pages, 5 figures. The lattice thermal conductivities, relaxation times and related quantities have been recalculated. Noticeable changes in results are for the clathrate structure VIII

References in corpus (4)

• Phonon-glass electron-crystal thermoelectric clathrates: Experiments and theory
• Impact of Rattlers on Thermal Conductivity of a Thermoelectric Clathrate: A First-Principles Study
• First-principles calculations of phonon frequencies, lifetimes and spectral functions from weak to strong anharmonicity: the example of palladium hydrides
• Ab initio lattice dynamical studies of silicon clathrate frameworks and their negative thermal expansion

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