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Nonequilibrium Phonon Dynamics and Its Impact on the Thermal Conductivity of the Benchmark Thermoelectric Material SnSe
KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.ORCID iD: 0000-0003-3851-5512
Uppsala Univ, Dept Phys & Astron, Mat Theory, S-75120 Uppsala, Sweden..
Uppsala Univ, Dept Phys & Astron, Mat Theory, S-75120 Uppsala, Sweden..ORCID iD: 0000-0001-5491-3962
Uppsala Univ, Dept Phys & Astron, Mat Theory, S-75120 Uppsala, Sweden..
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2023 (English)In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 17, no 21, p. 21006-21017Article in journal (Refereed) Published
Abstract [en]

Thermoelectric materials play a vital role in the pursuit of a sustainable energy system by allowing the conversion of waste heat to electric energy. Low thermal conductivity is essential to achieving high-efficiency conversion. The conductivity depends on an interplay between the phononic and electronic properties of the nonequilibrium state. Therefore, obtaining a comprehensive understanding of nonequilibrium dynamics of the electronic and phononic subsystems as well as their interactions is key for unlocking the microscopic mechanisms that ultimately govern thermal conductivity. A benchmark material that exhibits ultralow thermal conductivity is SnSe. We study the nonequilibrium phonon dynamics induced by an excited electron population using a framework combining ultrafast electron diffuse scattering and nonequilibrium kinetic theory. This in-depth approach provides a fundamental understanding of energy transfer in the spatiotemporal domain. Our analysis explains the dynamics leading to the observed low thermal conductivity, which we attribute to a mode-dependent tendency to nonconservative phonon scattering. The results offer a penetrating perspective on energy transport in condensed matter with far-reaching implications for rational design of advanced materials with tailored thermal properties.

Place, publisher, year, edition, pages
American Chemical Society (ACS) , 2023. Vol. 17, no 21, p. 21006-21017
Keywords [en]
Photoinduced electron diffuse scattering (PDS), thermoelectric, nonequilibrium phonon dynamics, SnSe, Ultrafastelectron microscope (UEM), electron-phonon coupling, phonon-phonon scattering
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:kth:diva-340212DOI: 10.1021/acsnano.3c03827ISI: 001092796200001PubMedID: 37862596Scopus ID: 2-s2.0-85177103121OAI: oai:DiVA.org:kth-340212DiVA, id: diva2:1815881
Note

QC 20231130

Available from: 2023-11-30 Created: 2023-11-30 Last updated: 2023-11-30Bibliographically approved

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Prasad, Amit KumarJi, ShaozhengWeissenrieder, Jonas

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