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Title: Antisite Pairs Suppress the Thermal Conductivity of BAs

BAs was predicted to have an unusually high thermal conductivity with a room temperature value of 2000 W m –1 K –1, comparable to that of diamond. However, the experimentally measured thermal conductivity of BAs single crystals is still lower than this value. To identify the origin of this large inconsistency, we investigate the lattice structure and potential defects in BAs single crystals at the atomic scale using aberration-corrected scanning transmission electron microscopy (STEM). Rather than finding a large concentration of As vacancies ( V As), as widely thought to dominate the thermal resistance in BAs, our STEM results show an enhanced intensity of some B columns and a reduced intensity of some As columns, suggesting the presence of antisite defects with As B (As atom on a B site) and B As (B atom on an As site). Additional calculations show that the antisite pair with As B next to B As is preferred energetically among the different types of point defects investigated and confirm that such defects lower the thermal conductivity for B As. Using a concentration of 1.8(8)% (6.6 ± 3.0 × 10 20 cm –3 in density) for the antisite pairs estimated from STEM images, themore » thermal conductivity is estimated to be 65–100 W m –1 K –1, in reasonable agreement with our measured value. Our study suggests that As B–B As antisite pairs are the primary lattice defects suppressing thermal conductivity of B As. Possible approaches are proposed for the growth of high-quality crystals or films with high thermal conductivity. In conclusion by employing a combination of state-of-the-art synthesis, STEM characterization, theory, and physical insight, this work models a path toward identifying and understanding defect-limited material functionality.« less
Authors:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 121; Journal Issue: 10; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1474871
Alternate Identifier(s):
OSTI ID: 1468867

Zheng, Qiang, Polanco, Carlos A., Du, Mao -Hua, Lindsay, Lucas R., Chi, Miaofang, Yan, Jiaqiang, and Sales, Brian C.. Antisite Pairs Suppress the Thermal Conductivity of BAs. United States: N. p., Web. doi:10.1103/PhysRevLett.121.105901.
Zheng, Qiang, Polanco, Carlos A., Du, Mao -Hua, Lindsay, Lucas R., Chi, Miaofang, Yan, Jiaqiang, & Sales, Brian C.. Antisite Pairs Suppress the Thermal Conductivity of BAs. United States. doi:10.1103/PhysRevLett.121.105901.
Zheng, Qiang, Polanco, Carlos A., Du, Mao -Hua, Lindsay, Lucas R., Chi, Miaofang, Yan, Jiaqiang, and Sales, Brian C.. 2018. "Antisite Pairs Suppress the Thermal Conductivity of BAs". United States. doi:10.1103/PhysRevLett.121.105901.
@article{osti_1474871,
title = {Antisite Pairs Suppress the Thermal Conductivity of BAs},
author = {Zheng, Qiang and Polanco, Carlos A. and Du, Mao -Hua and Lindsay, Lucas R. and Chi, Miaofang and Yan, Jiaqiang and Sales, Brian C.},
abstractNote = {BAs was predicted to have an unusually high thermal conductivity with a room temperature value of 2000 W m–1 K–1, comparable to that of diamond. However, the experimentally measured thermal conductivity of BAs single crystals is still lower than this value. To identify the origin of this large inconsistency, we investigate the lattice structure and potential defects in BAs single crystals at the atomic scale using aberration-corrected scanning transmission electron microscopy (STEM). Rather than finding a large concentration of As vacancies (VAs), as widely thought to dominate the thermal resistance in BAs, our STEM results show an enhanced intensity of some B columns and a reduced intensity of some As columns, suggesting the presence of antisite defects with AsB (As atom on a B site) and BAs (B atom on an As site). Additional calculations show that the antisite pair with AsB next to BAs is preferred energetically among the different types of point defects investigated and confirm that such defects lower the thermal conductivity for BAs. Using a concentration of 1.8(8)% (6.6 ± 3.0 × 1020 cm–3 in density) for the antisite pairs estimated from STEM images, the thermal conductivity is estimated to be 65–100 W m–1 K–1, in reasonable agreement with our measured value. Our study suggests that AsB–BAs antisite pairs are the primary lattice defects suppressing thermal conductivity of BAs. Possible approaches are proposed for the growth of high-quality crystals or films with high thermal conductivity. In conclusion by employing a combination of state-of-the-art synthesis, STEM characterization, theory, and physical insight, this work models a path toward identifying and understanding defect-limited material functionality.},
doi = {10.1103/PhysRevLett.121.105901},
journal = {Physical Review Letters},
number = 10,
volume = 121,
place = {United States},
year = {2018},
month = {9}
}

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