Anharmonicity in the High-Temperature Phase of SnSe: Soft Modes and Three-Phonon Interactions

JM Skelton, LA Burton, SC Parker, A Walsh, CE Kim… - Physical review …, 2016 - APS
Physical review letters, 2016APS
The layered semiconductor SnSe is one of the highest-performing thermoelectric materials
known. We demonstrate, through a first-principles lattice-dynamics study, that the high-
temperature C mcm phase is a dynamic average over lower-symmetry minima separated by
very small energetic barriers. Compared to the low-temperature P nma phase, the C mcm
phase displays a phonon softening and enhanced three-phonon scattering, leading to an
anharmonic damping of the low-frequency modes and hence the thermal transport. We …
The layered semiconductor SnSe is one of the highest-performing thermoelectric materials known. We demonstrate, through a first-principles lattice-dynamics study, that the high-temperature phase is a dynamic average over lower-symmetry minima separated by very small energetic barriers. Compared to the low-temperature phase, the phase displays a phonon softening and enhanced three-phonon scattering, leading to an anharmonic damping of the low-frequency modes and hence the thermal transport. We develop a renormalization scheme to quantify the effect of the soft modes on the calculated properties, and confirm that the anharmonicity is an inherent feature of the phase. These results suggest a design concept for thermal insulators and thermoelectric materials, based on displacive instabilities, and highlight the power of lattice-dynamics calculations for materials characterization.
American Physical Society