The origin of the lattice thermal conductivity enhancement at the ferroelectric phase transition in GeTe

D Dangic and O Hellman and S Fahy and I Savic, NPJ COMPUTATIONAL MATERIALS, 7, 57 (2021).

DOI: 10.1038/s41524-021-00523-7

The proximity to structural phase transitions in IV-VI thermoelectric materials is one of the main reasons for their large phonon anharmonicity and intrinsically low lattice thermal conductivity kappa. However, the kappa of GeTe increases at the ferroelectric phase transition near 700 K. Using first-principles calculations with the temperature dependent effective potential method, we show that this rise in kappa is the consequence of negative thermal expansion in the rhombohedral phase and increase in the phonon lifetimes in the high- symmetry phase. Strong anharmonicity near the phase transition induces non-Lorentzian shapes of the phonon power spectra. To account for these effects, we implement a method of calculating kappa based on the Green- Kubo approach and find that the Boltzmann transport equation underestimates kappa near the phase transition. Our findings elucidate the influence of structural phase transitions on kappa and provide guidance for design of better thermoelectric materials.

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