Strong Scattering from Low-Frequency Rattling Modes Results in Low Thermal Conductivity in Antimonide Clathrate Compounds

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Autor(es): dc.contributorColorado School of Mines-
Autor(es): dc.contributorPolish Academy of Sciences-
Autor(es): dc.contributorUniversity of California-
Autor(es): dc.contributorUniversidade Estadual Paulista (UNESP)-
Autor(es): dc.contributorUniversity of Illinois Urbana−Champaign-
Autor(es): dc.creatorCiesielski, Kamil M.-
Autor(es): dc.creatorOrtiz, Brenden R.-
Autor(es): dc.creatorGomes, Lidia C.-
Autor(es): dc.creatorMeschke, Vanessa-
Autor(es): dc.creatorAdamczyk, Jesse-
Autor(es): dc.creatorBraden, Tara L.-
Autor(es): dc.creatorKaczorowski, Dariusz-
Autor(es): dc.creatorErtekin, Elif-
Autor(es): dc.creatorToberer, Eric S.-
Data de aceite: dc.date.accessioned2025-08-21T15:28:35Z-
Data de disponibilização: dc.date.available2025-08-21T15:28:35Z-
Data de envio: dc.date.issued2023-07-29-
Data de envio: dc.date.issued2023-07-29-
Data de envio: dc.date.issued2023-04-11-
Fonte completa do material: dc.identifierhttp://dx.doi.org/10.1021/acs.chemmater.2c03821-
Fonte completa do material: dc.identifierhttp://hdl.handle.net/11449/248605-
Fonte: dc.identifier.urihttp://educapes.capes.gov.br/handle/11449/248605-
Descrição: dc.descriptionRecent discoveries of materials with ultralow thermal conductivity open a pathway to significant developments in the field of thermoelectricity. Here, we conduct a comparative study of three chemically similar antimonides to establish the root causes of their extraordinarily low thermal conductivity (0.4-0.6 W m-1 K-1 at 525 K). The materials of interest are the unconventional type-XI clathrate K58Zn122Sb207, the tunnel compound K6.9Zn21Sb16, and the type-I clathrate K8Zn15.5Cu2.5Sb28 discovered herein. Calculations of the phonon dispersions show that the type-XI compound exhibits localized (i.e., rattling) phonon modes with unusually low frequencies that span the entire acoustic regime. In contrast, rattling in type I clathrate is observed only at higher frequencies, and no rattling modes are present in the tunnel structure. Modeling reveals that low-frequency rattling modes profoundly limit the acoustic scattering time; the scattering time of the type-XI clathrate is half that of the type-I clathrate and a quarter of that of the tunnel compound. For all three materials, the thermal conductivities are additionally suppressed by soft framework bonding that lowers the acoustic group velocities and structural complexity that leads to diffusonic character of the optical modes. Understanding the details of thermal transport in structurally complex materials will be crucial for developing the next generation of thermoelectrics.-
Descrição: dc.descriptionDivision of Materials Research-
Descrição: dc.descriptionNational Science Foundation-
Descrição: dc.descriptionNational Sleep Foundation-
Descrição: dc.descriptionNational Stroke Foundation-
Descrição: dc.descriptionNorsk Sykepleierforbund-
Descrição: dc.descriptionDepartment of Physics Colorado School of Mines-
Descrição: dc.descriptionInstitute of Low Temperature and Structure Research Polish Academy of Sciences-
Descrição: dc.descriptionMaterials Department University of California-
Descrição: dc.descriptionInstituto de Física Teórica São Paulo State University (UNESP), São Paulo-
Descrição: dc.descriptionCentre for Advanced Materials and Smart Structures Polish Academy of Sciences-
Descrição: dc.descriptionDepartment of Mechanical Science and Engineering University of Illinois Urbana−Champaign-
Descrição: dc.descriptionInstituto de Física Teórica São Paulo State University (UNESP), São Paulo-
Formato: dc.format2918-2935-
Idioma: dc.languageen-
Relação: dc.relationChemistry of Materials-
???dc.source???: dc.sourceScopus-
Título: dc.titleStrong Scattering from Low-Frequency Rattling Modes Results in Low Thermal Conductivity in Antimonide Clathrate Compounds-
Tipo de arquivo: dc.typelivro digital-
Aparece nas coleções:Repositório Institucional - Unesp

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