Lattice thermal conductivity in the anharmonic overdamped regime

In crystalline materials, low lattice thermal conductivity is often associated with strong anharmonicity, causing significant deviations from the expected Lorentzian lineshape of phonon spectral functions. These deviations, occurring in an overdamped regime, raise questions about the applicability o...

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Autores: Dangic, Dorde, Caldarelli, Giovanni, Bianco, Raffaello, Savić, Ivana, Errea Lope, Ion
Tipo de recurso: artículo
Fecha de publicación:2025
País:España
Institución:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/73105
Acceso en línea:http://hdl.handle.net/10810/73105
Access Level:acceso abierto
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spelling Lattice thermal conductivity in the anharmonic overdamped regimeDangic, DordeCaldarelli, GiovanniBianco, RaffaelloSavić, IvanaErrea Lope, IonIn crystalline materials, low lattice thermal conductivity is often associated with strong anharmonicity, causing significant deviations from the expected Lorentzian lineshape of phonon spectral functions. These deviations, occurring in an overdamped regime, raise questions about the applicability of the Boltzmann transport equation. Furthermore, strong anharmonicity can trigger structural phase transitions with temperature that cannot be adequately described by the standard harmonic approximation. To address these challenges, we propose an approach for computing lattice thermal conductivity. Our method combines the Green-Kubo linear response theory with the stochastic self-consistent harmonic approximation. The latter describes the temperature-dependent evolution of the crystal structure, including first- and second-order phase transitions, as well as the vibrational properties in highly anharmonic materials. The Green-Kubo method considers the full lineshapes of phonon spectral functions in the calculation of lattice thermal conductivity, thus eliminating the questionable use of phonon lifetimes in the overdamped regime and naturally including coherent transport effects. Additionally, we extend our theory to model complex dynamical lattice thermal conductivity, enhancing understanding of time-dependent thermoreflectance experiments. As a practical application, we employ this approach to calculate lattice thermal conductivity of CsPbBr3, a complex crystal known for its anomalous thermal transport behavior and a complex phase diagram. Our method determines the thermal conductivity across different phases in good agreement with experiments.This work was supported by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant Agreement No. 802533), the Spanish Ministry of Science and Innovation (Grant No. PID2022-142861NA-I00), and the Department of Education, Universities and Research of the Eusko Jaurlaritza and the University of the Basque Country UPV/EHU (Grant No. IT1527-22).APSEuropean Commission202520252025info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10810/73105reponame:Addi. Archivo Digital para la Docencia y la Investigacióninstname:Universidad del País VascoInglésinfo:eu-repo/grantAgreement/EC/H2020/802533info:eu-repo/grantAgreement/MCIN/PID2022-142861NA-I00/https://doi.org/10.1103/PhysRevB.111.104314info:eu-repo/semantics/openAccess© 2025 American Physical Societyoai:addi.ehu.eus:10810/731052026-06-18T09:23:17Z
dc.title.none.fl_str_mv Lattice thermal conductivity in the anharmonic overdamped regime
title Lattice thermal conductivity in the anharmonic overdamped regime
spellingShingle Lattice thermal conductivity in the anharmonic overdamped regime
Dangic, Dorde
title_short Lattice thermal conductivity in the anharmonic overdamped regime
title_full Lattice thermal conductivity in the anharmonic overdamped regime
title_fullStr Lattice thermal conductivity in the anharmonic overdamped regime
title_full_unstemmed Lattice thermal conductivity in the anharmonic overdamped regime
title_sort Lattice thermal conductivity in the anharmonic overdamped regime
dc.creator.none.fl_str_mv Dangic, Dorde
Caldarelli, Giovanni
Bianco, Raffaello
Savić, Ivana
Errea Lope, Ion
author Dangic, Dorde
author_facet Dangic, Dorde
Caldarelli, Giovanni
Bianco, Raffaello
Savić, Ivana
Errea Lope, Ion
author_role author
author2 Caldarelli, Giovanni
Bianco, Raffaello
Savić, Ivana
Errea Lope, Ion
author2_role author
author
author
author
dc.contributor.none.fl_str_mv European Commission
description In crystalline materials, low lattice thermal conductivity is often associated with strong anharmonicity, causing significant deviations from the expected Lorentzian lineshape of phonon spectral functions. These deviations, occurring in an overdamped regime, raise questions about the applicability of the Boltzmann transport equation. Furthermore, strong anharmonicity can trigger structural phase transitions with temperature that cannot be adequately described by the standard harmonic approximation. To address these challenges, we propose an approach for computing lattice thermal conductivity. Our method combines the Green-Kubo linear response theory with the stochastic self-consistent harmonic approximation. The latter describes the temperature-dependent evolution of the crystal structure, including first- and second-order phase transitions, as well as the vibrational properties in highly anharmonic materials. The Green-Kubo method considers the full lineshapes of phonon spectral functions in the calculation of lattice thermal conductivity, thus eliminating the questionable use of phonon lifetimes in the overdamped regime and naturally including coherent transport effects. Additionally, we extend our theory to model complex dynamical lattice thermal conductivity, enhancing understanding of time-dependent thermoreflectance experiments. As a practical application, we employ this approach to calculate lattice thermal conductivity of CsPbBr3, a complex crystal known for its anomalous thermal transport behavior and a complex phase diagram. Our method determines the thermal conductivity across different phases in good agreement with experiments.
publishDate 2025
dc.date.none.fl_str_mv 2025
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10810/73105
url http://hdl.handle.net/10810/73105
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/EC/H2020/802533
info:eu-repo/grantAgreement/MCIN/PID2022-142861NA-I00/
https://doi.org/10.1103/PhysRevB.111.104314
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
© 2025 American Physical Society
eu_rights_str_mv openAccess
rights_invalid_str_mv © 2025 American Physical Society
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv APS
publisher.none.fl_str_mv APS
dc.source.none.fl_str_mv reponame:Addi. Archivo Digital para la Docencia y la Investigación
instname:Universidad del País Vasco
instname_str Universidad del País Vasco
reponame_str Addi. Archivo Digital para la Docencia y la Investigación
collection Addi. Archivo Digital para la Docencia y la Investigación
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