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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 ( BaAb 2SnSe 4, BaCu 2GeSe 4, BaCu 2SnSe 4 and SrCu 2GeSe 4) with experimentally-measured thermal conductivity as low as 0.31 ± 0.03 W m -1 K -1 at 673 K for BaAg 2SnSe 4. Density functional theory calculations predict κ < 0.3 W m -1 K -1 for BaAg 2SnSe 4 due to scattering from weakly-bonded Ag–Ag dimers. Lastly, 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.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [5]; ORCiD logo [6];  [7]; ORCiD logo [8]; ORCiD logo [7]; ORCiD logo [7];  [6]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
  2. Koç Univ., Sariyer (Turkey). Dept. of Chemistry
  3. Dalhousie Univ., Halifax (Canada). Dept. of Physics and Atmospheric Science
  4. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physical and Life Sciences Directorate
  5. Univ. Catholique de Louvain, Louvain-la-Neuve (Belgium). Inst. of Condensed Matter and Nanosciences (IMCN); Wuhan Univ. (China). School of Physics and Technology
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Technologies Area
  7. Univ. Catholique de Louvain, Louvain-la-Neuve (Belgium). Inst. of Condensed Matter and Nanosciences (IMCN)
  8. Dalhousie Univ., Halifax (Canada). Dept. of Physics and Atmospheric Science, Clean Technologies Research Inst., and Dept. of Chemistry
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); Dalhousie Research in Energy, Advanced Materials and Sustainability (DREAMS); NSERC CREATE
OSTI Identifier:
1497956
Report Number(s):
LLNL-JRNL-759504
Journal ID: ISSN 2050-7488; JMCAET; 947508
Grant/Contract Number:  
AC52-07NA27344; AC02-05CH11231; 1334713; 1334351; 1333335
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 7; Journal Issue: 6; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Kuo, Jimmy Jiahong, Aydemir, Umut, Pöhls, Jan-Hendrik, Zhou, Fei, Yu, Guodong, Faghaninia, Alireza, Ricci, Francesco, White, Mary Anne, Rignanese, Gian-Marco, Hautier, Geoffroy, Jain, Anubhav, and Snyder, G. Jeffrey. Origins of ultralow thermal conductivity in 1-2-1-4 quaternary selenides. United States: N. p., 2019. Web. doi:10.1039/c8ta09660k.
Kuo, Jimmy Jiahong, Aydemir, Umut, Pöhls, Jan-Hendrik, Zhou, Fei, Yu, Guodong, Faghaninia, Alireza, Ricci, Francesco, White, Mary Anne, Rignanese, Gian-Marco, Hautier, Geoffroy, Jain, Anubhav, & Snyder, G. Jeffrey. Origins of ultralow thermal conductivity in 1-2-1-4 quaternary selenides. United States. doi:10.1039/c8ta09660k.
Kuo, Jimmy Jiahong, Aydemir, Umut, Pöhls, Jan-Hendrik, Zhou, Fei, Yu, Guodong, Faghaninia, Alireza, Ricci, Francesco, White, Mary Anne, Rignanese, Gian-Marco, Hautier, Geoffroy, Jain, Anubhav, and Snyder, G. Jeffrey. Mon . "Origins of ultralow thermal conductivity in 1-2-1-4 quaternary selenides". United States. doi:10.1039/c8ta09660k.
@article{osti_1497956,
title = {Origins of ultralow thermal conductivity in 1-2-1-4 quaternary selenides},
author = {Kuo, Jimmy Jiahong and Aydemir, Umut and Pöhls, Jan-Hendrik and Zhou, Fei and Yu, Guodong and Faghaninia, Alireza and Ricci, Francesco and White, Mary Anne and Rignanese, Gian-Marco and Hautier, Geoffroy and Jain, Anubhav and Snyder, G. Jeffrey},
abstractNote = {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 ( BaAb2SnSe4, BaCu2GeSe4, BaCu2SnSe4 and SrCu2GeSe4) with experimentally-measured thermal conductivity as low as 0.31 ± 0.03 W m-1 K-1 at 673 K for BaAg2SnSe4. Density functional theory calculations predict κ < 0.3 W m-1 K-1 for BaAg2SnSe4 due to scattering from weakly-bonded Ag–Ag dimers. Lastly, 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.},
doi = {10.1039/c8ta09660k},
journal = {Journal of Materials Chemistry. A},
number = 6,
volume = 7,
place = {United States},
year = {2019},
month = {1}
}

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