Origins of ultralow thermal conductivity in 1-2-1-4 quaternary selenides

Jimmy Jiahong Kuo; Umut Aydemir; Jan Hendrik Pöhls; Fei Zhou; Guodong Yu; Alireza Faghaninia; Francesco Ricci; Mary Anne White; Gian Marco Rignanese; Geoffroy Hautier; Anubhav Jain; G. Jeffrey Snyder

doi:10.1039/c8ta09660k

Origins of ultralow thermal conductivity in 1-2-1-4 quaternary selenides

Jimmy Jiahong Kuo, Umut Aydemir, Jan Hendrik Pöhls, Fei Zhou, Guodong Yu, Alireza Faghaninia, Francesco Ricci, Mary Anne White, Gian Marco Rignanese, Geoffroy Hautier, Anubhav Jain, G. Jeffrey Snyder^*

^*Corresponding author for this work

Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

21 Scopus citations

Abstract

Engineering the thermal properties in solids is important for both fundamental physics (e.g. electric and phonon transport) and device applications (e.g. thermal insulating coating, thermoelectrics). In this paper, we report low thermal transport properties of four selenide compounds (BaAg ₂ SnSe ₄ , BaCu ₂ GeSe ₄ , BaCu ₂ SnSe ₄ and SrCu ₂ GeSe ₄ ) with experimentally-measured thermal conductivity as low as 0.31 ± 0.03 W m ^-1 K ^-1 at 673 K for BaAg ₂ SnSe ₄ . Density functional theory calculations predict κ < 0.3 W m ^-1 K ^-1 for BaAg ₂ SnSe ₄ due to scattering from weakly-bonded Ag-Ag dimers. Defect calculations suggest that achieving high hole doping levels in these materials could be challenging due to monovalent (e.g., Ag) interstitials acting as hole killers, resulting in overall low electrical conductivity in these compounds.

Original language	English (US)
Pages (from-to)	2589-2596
Number of pages	8
Journal	Journal of Materials Chemistry A
Volume	7
Issue number	6
DOIs	https://doi.org/10.1039/c8ta09660k
State	Published - 2019

ASJC Scopus subject areas

Chemistry(all)
Renewable Energy, Sustainability and the Environment
Materials Science(all)

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@article{ec8c5df52dd64cb09e22b1ec22ca1ff9,

title = "Origins of ultralow thermal conductivity in 1-2-1-4 quaternary selenides",

abstract = " Engineering the thermal properties in solids is important for both fundamental physics (e.g. electric and phonon transport) and device applications (e.g. thermal insulating coating, thermoelectrics). In this paper, we report low thermal transport properties of four selenide compounds (BaAg 2 SnSe 4 , BaCu 2 GeSe 4 , BaCu 2 SnSe 4 and SrCu 2 GeSe 4 ) with experimentally-measured thermal conductivity as low as 0.31 ± 0.03 W m -1 K -1 at 673 K for BaAg 2 SnSe 4 . Density functional theory calculations predict κ < 0.3 W m -1 K -1 for BaAg 2 SnSe 4 due to scattering from weakly-bonded Ag-Ag dimers. Defect calculations suggest that achieving high hole doping levels in these materials could be challenging due to monovalent (e.g., Ag) interstitials acting as hole killers, resulting in overall low electrical conductivity in these compounds.",

author = "Kuo, {Jimmy Jiahong} and Umut Aydemir and P{\"o}hls, {Jan Hendrik} and Fei Zhou and Guodong Yu and Alireza Faghaninia and Francesco Ricci and White, {Mary Anne} and Rignanese, {Gian Marco} and Geoffroy Hautier and Anubhav Jain and Snyder, {G. Jeffrey}",

note = "Funding Information: JK acknowledges NSF DMREF (grant no. 1334713, 1334351, and 1333335) for support of this research. AJ and AF were funded by the U.S. Department of Energy, Office of Basic Energy Sciences, Early Career Research Program (ECRP). FZ was supported by the Laboratory Directed Research and Development program at Lawrence Livermore National Laboratory and performed under the auspices of the U.S. Department of Energy by LLNL under Contract DE-AC52-07NA27344. This research used resources of the National Energy Research Scientic Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. JHP acknowledges support from Dalhousie Research in Energy, Advanced Materials and Sustainability (DREAMS), an NSERC CREATE program, and a Nova Scotia scholarship. MAW acknowledges support from NSERC and the Clean Technologies Research Institute at Dal-housie University. Publisher Copyright: {\textcopyright} 2019 The Royal Society of Chemistry.",

year = "2019",

doi = "10.1039/c8ta09660k",

language = "English (US)",

volume = "7",

pages = "2589--2596",

journal = "Journal of Materials Chemistry A",

issn = "2050-7488",

publisher = "Royal Society of Chemistry",

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T1 - Origins of ultralow thermal conductivity in 1-2-1-4 quaternary selenides

AU - Kuo, Jimmy Jiahong

AU - Aydemir, Umut

AU - Pöhls, Jan Hendrik

AU - Zhou, Fei

AU - Yu, Guodong

AU - Faghaninia, Alireza

AU - Ricci, Francesco

AU - White, Mary Anne

AU - Rignanese, Gian Marco

AU - Hautier, Geoffroy

AU - Jain, Anubhav

AU - Snyder, G. Jeffrey

N1 - Funding Information: JK acknowledges NSF DMREF (grant no. 1334713, 1334351, and 1333335) for support of this research. AJ and AF were funded by the U.S. Department of Energy, Office of Basic Energy Sciences, Early Career Research Program (ECRP). FZ was supported by the Laboratory Directed Research and Development program at Lawrence Livermore National Laboratory and performed under the auspices of the U.S. Department of Energy by LLNL under Contract DE-AC52-07NA27344. This research used resources of the National Energy Research Scientic Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. JHP acknowledges support from Dalhousie Research in Energy, Advanced Materials and Sustainability (DREAMS), an NSERC CREATE program, and a Nova Scotia scholarship. MAW acknowledges support from NSERC and the Clean Technologies Research Institute at Dal-housie University. Publisher Copyright: © 2019 The Royal Society of Chemistry.

PY - 2019

Y1 - 2019

N2 - Engineering the thermal properties in solids is important for both fundamental physics (e.g. electric and phonon transport) and device applications (e.g. thermal insulating coating, thermoelectrics). In this paper, we report low thermal transport properties of four selenide compounds (BaAg 2 SnSe 4 , BaCu 2 GeSe 4 , BaCu 2 SnSe 4 and SrCu 2 GeSe 4 ) with experimentally-measured thermal conductivity as low as 0.31 ± 0.03 W m -1 K -1 at 673 K for BaAg 2 SnSe 4 . Density functional theory calculations predict κ < 0.3 W m -1 K -1 for BaAg 2 SnSe 4 due to scattering from weakly-bonded Ag-Ag dimers. Defect calculations suggest that achieving high hole doping levels in these materials could be challenging due to monovalent (e.g., Ag) interstitials acting as hole killers, resulting in overall low electrical conductivity in these compounds.

AB - Engineering the thermal properties in solids is important for both fundamental physics (e.g. electric and phonon transport) and device applications (e.g. thermal insulating coating, thermoelectrics). In this paper, we report low thermal transport properties of four selenide compounds (BaAg 2 SnSe 4 , BaCu 2 GeSe 4 , BaCu 2 SnSe 4 and SrCu 2 GeSe 4 ) with experimentally-measured thermal conductivity as low as 0.31 ± 0.03 W m -1 K -1 at 673 K for BaAg 2 SnSe 4 . Density functional theory calculations predict κ < 0.3 W m -1 K -1 for BaAg 2 SnSe 4 due to scattering from weakly-bonded Ag-Ag dimers. Defect calculations suggest that achieving high hole doping levels in these materials could be challenging due to monovalent (e.g., Ag) interstitials acting as hole killers, resulting in overall low electrical conductivity in these compounds.

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U2 - 10.1039/c8ta09660k

DO - 10.1039/c8ta09660k

M3 - Article

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SN - 2050-7488

VL - 7

SP - 2589

EP - 2596

JO - Journal of Materials Chemistry A

JF - Journal of Materials Chemistry A

IS - 6

ER -

Origins of ultralow thermal conductivity in 1-2-1-4 quaternary selenides

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