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Nonequilibrium Phonon Dynamics and Its Impact on the Thermal Conductivity of the Benchmark Thermoelectric Material SnSe
KTH Royal Inst Technol, Sch Engn Sci, Mat & Nano Phys, SE-10044 Stockholm, Sweden..ORCID iD: 0000-0003-3851-5512
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.ORCID iD: 0000-0001-5491-3962
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.ORCID iD: 0000-0002-8524-819x
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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:uu:diva-516644DOI: 10.1021/acsnano.3c03827ISI: 001092796200001PubMedID: 37862596OAI: oai:DiVA.org:uu-516644DiVA, id: diva2:1815719
Funder
Knut and Alice Wallenberg Foundation, 2012.0321Swedish Research Council, VR 2021-00171Swedish Research Council, 2018-05973Swedish Research Council, 2019-03901Knut and Alice Wallenberg Foundation, 2018.0104Swedish National Infrastructure for Computing (SNIC)Swedish Foundation for Strategic Research, ICA16-0037EU, European Research Council, 854843Carl Tryggers foundation , CTS20:153Available from: 2023-11-29 Created: 2023-11-29 Last updated: 2023-11-29Bibliographically approved

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Sebesta, JakubEsteban-Puyuelo, RaquelMaldonado, PabloSanyal, BiplabGrånäs, Oscar

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