Cargando…
Layered Tin Chalcogenides SnS and SnSe: Lattice Thermal Conductivity Benchmarks and Thermoelectric Figure of Merit
[Image: see text] Tin sulfide (SnS) and tin selenide (SnSe) are attractive materials for thermoelectric conversion applications. Favorable small band gap, high carrier mobility, large Seebeck coefficient, and remarkably low lattice thermal conductivity are a consequence of their anisotropic crystal...
Autores principales: | , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2022
|
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9421910/ https://www.ncbi.nlm.nih.gov/pubmed/36051253 http://dx.doi.org/10.1021/acs.jpcc.2c02401 |
_version_ | 1784777700225843200 |
---|---|
author | Rundle, Jordan Leoni, Stefano |
author_facet | Rundle, Jordan Leoni, Stefano |
author_sort | Rundle, Jordan |
collection | PubMed |
description | [Image: see text] Tin sulfide (SnS) and tin selenide (SnSe) are attractive materials for thermoelectric conversion applications. Favorable small band gap, high carrier mobility, large Seebeck coefficient, and remarkably low lattice thermal conductivity are a consequence of their anisotropic crystal structure of symmetry Pnma, made of corrugated, black phosphorus-like layers. Their internal lattice dynamics combined with chemical bond softening in going from SnS to SnSe make for subtle effects on lattice thermal conductivity. Reliable prediction of phonon transport for these materials must therefore include many-body effects. Using first principles methods and a transferable tight-binding potential for frozen phonon calculations, here, we investigate the evolution of thermal lattice conductivity and thermoelectric figure of merit in Pnma-SnS and -SnSe, also including the high-temperature Cmcm-SnS phase. We show how thermal conductivity lowering in SnS at higher temperatures is largely due to dynamic phonon softening ahead of the Pnma–Cmcm structural phase transition. SnS becomes more similar to SnSe in its lifetime and mean free path profiles as it approaches its high-temperature Cmcm phase. The latter nonetheless intrinsically constraints phonon group velocity modules, preventing SnS to overtake SnSe. Our analysis provides important insights and computational benchmarks for optimization of thermoelectric materials via a more efficient computational strategy compared to previous ab initio attempts, one that can be easily transferred to larger systems for further thermoelectric materials nanoengineering. The good description of anharmonicity at higher temperatures inherent to the tight-binding potential yields calculated lattice conductivity values that are in very good agreement with experiments. |
format | Online Article Text |
id | pubmed-9421910 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-94219102022-08-30 Layered Tin Chalcogenides SnS and SnSe: Lattice Thermal Conductivity Benchmarks and Thermoelectric Figure of Merit Rundle, Jordan Leoni, Stefano J Phys Chem C Nanomater Interfaces [Image: see text] Tin sulfide (SnS) and tin selenide (SnSe) are attractive materials for thermoelectric conversion applications. Favorable small band gap, high carrier mobility, large Seebeck coefficient, and remarkably low lattice thermal conductivity are a consequence of their anisotropic crystal structure of symmetry Pnma, made of corrugated, black phosphorus-like layers. Their internal lattice dynamics combined with chemical bond softening in going from SnS to SnSe make for subtle effects on lattice thermal conductivity. Reliable prediction of phonon transport for these materials must therefore include many-body effects. Using first principles methods and a transferable tight-binding potential for frozen phonon calculations, here, we investigate the evolution of thermal lattice conductivity and thermoelectric figure of merit in Pnma-SnS and -SnSe, also including the high-temperature Cmcm-SnS phase. We show how thermal conductivity lowering in SnS at higher temperatures is largely due to dynamic phonon softening ahead of the Pnma–Cmcm structural phase transition. SnS becomes more similar to SnSe in its lifetime and mean free path profiles as it approaches its high-temperature Cmcm phase. The latter nonetheless intrinsically constraints phonon group velocity modules, preventing SnS to overtake SnSe. Our analysis provides important insights and computational benchmarks for optimization of thermoelectric materials via a more efficient computational strategy compared to previous ab initio attempts, one that can be easily transferred to larger systems for further thermoelectric materials nanoengineering. The good description of anharmonicity at higher temperatures inherent to the tight-binding potential yields calculated lattice conductivity values that are in very good agreement with experiments. American Chemical Society 2022-08-16 2022-08-25 /pmc/articles/PMC9421910/ /pubmed/36051253 http://dx.doi.org/10.1021/acs.jpcc.2c02401 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Rundle, Jordan Leoni, Stefano Layered Tin Chalcogenides SnS and SnSe: Lattice Thermal Conductivity Benchmarks and Thermoelectric Figure of Merit |
title | Layered Tin Chalcogenides
SnS and SnSe: Lattice Thermal
Conductivity Benchmarks and Thermoelectric Figure of Merit |
title_full | Layered Tin Chalcogenides
SnS and SnSe: Lattice Thermal
Conductivity Benchmarks and Thermoelectric Figure of Merit |
title_fullStr | Layered Tin Chalcogenides
SnS and SnSe: Lattice Thermal
Conductivity Benchmarks and Thermoelectric Figure of Merit |
title_full_unstemmed | Layered Tin Chalcogenides
SnS and SnSe: Lattice Thermal
Conductivity Benchmarks and Thermoelectric Figure of Merit |
title_short | Layered Tin Chalcogenides
SnS and SnSe: Lattice Thermal
Conductivity Benchmarks and Thermoelectric Figure of Merit |
title_sort | layered tin chalcogenides
sns and snse: lattice thermal
conductivity benchmarks and thermoelectric figure of merit |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9421910/ https://www.ncbi.nlm.nih.gov/pubmed/36051253 http://dx.doi.org/10.1021/acs.jpcc.2c02401 |
work_keys_str_mv | AT rundlejordan layeredtinchalcogenidessnsandsnselatticethermalconductivitybenchmarksandthermoelectricfigureofmerit AT leonistefano layeredtinchalcogenidessnsandsnselatticethermalconductivitybenchmarksandthermoelectricfigureofmerit |