Antisite Pairs Suppress the Thermal Conductivity of BAs

Zheng, Qiang; Polanco, Carlos A.; Du, Mao -Hua; Lindsay, Lucas R.; Chi, Miaofang; Yan, Jiaqiang; Sales, Brian C.

doi:10.1103/PhysRevLett.121.105901

Title: Antisite Pairs Suppress the Thermal Conductivity of BAs

Journal Article · 06 September 2018 · Physical Review Letters

DOI: https://doi.org/10.1103/PhysRevLett.121.105901 · OSTI ID:1474871

^[1];

^[2];

^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

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 × 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 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.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1474871

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 10 Vol. 121; ISSN 0031-9007; ISSN PRLTAO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (48)

EELS log-ratio technique for specimen-thickness measurement in the TEM Malis, T.; Cheng, S. C.; Egerton, R. F. Journal of Electron Microscopy Technique, Vol. 8, Issue 2 https://doi.org/10.1002/jemt.1060080206	journal	February 1988
Electron Energy-Loss Spectroscopy in the Electron Microscope Egerton, R. F. https://doi.org/10.1007/978-1-4419-9583-4	book	January 2011
Electron Energy-Loss Spectroscopy in the Electron Microscope Egerton, Ray F. Springer New York, NY https://doi.org/10.1007/978-1-4615-6887-2	book	January 1995
Phase diagram of the system nickel-boron Portnoi, K. I.; Romashov, V. M.; Chubarov, V. M. Soviet Powder Metallurgy and Metal Ceramics, Vol. 6, Issue 2 https://doi.org/10.1007/BF00775639	journal	February 1967
The crystal structure of the ф phase in the boron-sodium system Naslain, Roger; Kasper, John S. Journal of Solid State Chemistry, Vol. 1, Issue 2 https://doi.org/10.1016/0022-4596(70)90006-X	journal	January 1970
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Semiconducting icosahedral boron arsenide crystal growth for neutron detection Whiteley, C. E.; Zhang, Y.; Gong, Y. Journal of Crystal Growth, Vol. 318, Issue 1 https://doi.org/10.1016/j.jcrysgro.2010.10.057	journal	March 2011
Emerging challenges and materials for thermal management of electronics Moore, Arden L.; Shi, Li Materials Today, Vol. 17, Issue 4 https://doi.org/10.1016/j.mattod.2014.04.003	journal	May 2014
An electron microscope for the aberration-corrected era Krivanek, O. L.; Corbin, G. J.; Dellby, N. Ultramicroscopy, Vol. 108, Issue 3 https://doi.org/10.1016/j.ultramic.2007.07.010	journal	February 2008
Effects of electron channeling in HAADF-STEM intensity in La2CuSnO6 Haruta, M.; Kurata, H.; Komatsu, H. Ultramicroscopy, Vol. 109, Issue 4 https://doi.org/10.1016/j.ultramic.2009.01.004	journal	March 2009
Thermal Properties and Phonon Spectral Characterization of Synthetic Boron Phosphide for High Thermal Conductivity Applications Kang, Joon Sang; Wu, Huan; Hu, Yongjie Nano Letters, Vol. 17, Issue 12 https://doi.org/10.1021/acs.nanolett.7b03437	journal	November 2017
Thermal conductivity of isotopically modified graphene Chen, Shanshan; Wu, Qingzhi; Mishra, Columbia Nature Materials, Vol. 11, Issue 3 https://doi.org/10.1038/nmat3207	journal	January 2012
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets Chen, Ruyi; Cui, Qirui; Liao, Liyang Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23414-3	journal	May 2021
High-resolution X-ray luminescence extension imaging Ou, Xiangyu; Qin, Xian; Huang, Bolong Nature, Vol. 590, Issue 7846 https://doi.org/10.1038/s41586-021-03251-6	journal	February 2021
Hybrid functionals based on a screened Coulomb potential Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 118, Issue 18 https://doi.org/10.1063/1.1564060	journal	May 2003
Crystal Growth and Properties of Boron Monoarsenide Chu, T. L.; Hyslop, A. E. Journal of Applied Physics, Vol. 43, Issue 2 https://doi.org/10.1063/1.1661106	journal	February 1972
Influence of the exchange screening parameter on the performance of screened hybrid functionals Krukau, Aliaksandr V.; Vydrov, Oleg A.; Izmaylov, Artur F. The Journal of Chemical Physics, Vol. 125, Issue 22 https://doi.org/10.1063/1.2404663	journal	December 2006
Experimental study of the proposed super-thermal-conductor: BAs Lv, Bing; Lan, Yucheng; Wang, Xiqu Applied Physics Letters, Vol. 106, Issue 7 https://doi.org/10.1063/1.4913441	journal	February 2015
Thermal and thermoelectric transport measurements of an individual boron arsenide microstructure Kim, Jaehyun; Evans, Daniel A.; Sellan, Daniel P. Applied Physics Letters, Vol. 108, Issue 20 https://doi.org/10.1063/1.4950970	journal	May 2016
Seeded growth of boron arsenide single crystals with high thermal conductivity Tian, Fei; Song, Bai; Lv, Bing Applied Physics Letters, Vol. 112, Issue 3 https://doi.org/10.1063/1.5004200	journal	January 2018
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
Electrons and Phonons Ziman, J. M. https://doi.org/10.1093/acprof:oso/9780198507796.001.0001	book	January 2001
Self-interaction correction to density-functional approximations for many-electron systems Perdew, J. P.; Zunger, Alex Physical Review B, Vol. 23, Issue 10, p. 5048-5079 https://doi.org/10.1103/PhysRevB.23.5048	journal	May 1981
Thermal diffusivity of isotopically enriched C 12 diamond Anthony, T. R.; Banholzer, W. F.; Fleischer, J. F. Physical Review B, Vol. 42, Issue 2 https://doi.org/10.1103/PhysRevB.42.1104	journal	July 1990
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Method to extract anharmonic force constants from first principles calculations Esfarjani, Keivan; Stokes, Harold T. Physical Review B, Vol. 77, Issue 14 https://doi.org/10.1103/PhysRevB.77.144112	journal	April 2008
Assessment of correction methods for the band-gap problem and for finite-size effects in supercell defect calculations: Case studies for ZnO and GaAs Lany, Stephan; Zunger, Alex Physical Review B, Vol. 78, Issue 23, Article No. 235104 https://doi.org/10.1103/PhysRevB.78.235104	journal	December 2008
Cluster scattering effects on phonon conduction in graphene Mingo, Natalio; Esfarjani, K.; Broido, D. A. Physical Review B, Vol. 81, Issue 4 https://doi.org/10.1103/PhysRevB.81.045408	journal	January 2010
Electronic structure and defect properties of Tl 6 SeI 4 : Density functional calculations Biswas, Koushik; Du, Mao-Hua; Singh, David J. Physical Review B, Vol. 86, Issue 14 https://doi.org/10.1103/PhysRevB.86.144108	journal	October 2012
Ab initio thermal transport in compound semiconductors Lindsay, L.; Broido, D. A.; Reinecke, T. L. Physical Review B, Vol. 87, Issue 16 https://doi.org/10.1103/PhysRevB.87.165201	journal	April 2013
Ab initio study of the unusual thermal transport properties of boron arsenide and related materials Broido, D. A.; Lindsay, L.; Reinecke, T. L. Physical Review B, Vol. 88, Issue 21 https://doi.org/10.1103/PhysRevB.88.214303	journal	December 2013
Effect of nitrogen and vacancy defects on the thermal conductivity of diamond: An ab initio Green's function approach Katcho, N. A.; Carrete, J.; Li, Wu Physical Review B, Vol. 90, Issue 9 https://doi.org/10.1103/PhysRevB.90.094117	journal	September 2014
Ab initio study of the effect of vacancies on the thermal conductivity of boron arsenide Protik, Nakib Haider; Carrete, Jesús; Katcho, Nebil A. Physical Review B, Vol. 94, Issue 4 https://doi.org/10.1103/PhysRevB.94.045207	journal	July 2016
Boron arsenide phonon dispersion from inelastic x-ray scattering: Potential for ultrahigh thermal conductivity Ma, Hao; Li, Chen; Tang, Shixiong Physical Review B, Vol. 94, Issue 22 https://doi.org/10.1103/PhysRevB.94.220303	journal	December 2016
First-principles prediction of stabilities and instabilities of compounds and alloys in the ternary B-As-P system Ektarawong, A.; Simak, S. I.; Alling, B. Physical Review B, Vol. 96, Issue 2 https://doi.org/10.1103/PhysRevB.96.024202	journal	July 2017
Ab initio phonon point defect scattering and thermal transport in graphene Polanco, Carlos A.; Lindsay, Lucas Physical Review B, Vol. 97, Issue 1 https://doi.org/10.1103/PhysRevB.97.014303	journal	January 2018
First-Principles Determination of Ultrahigh Thermal Conductivity of Boron Arsenide: A Competitor for Diamond? Lindsay, L.; Broido, D. A.; Reinecke, T. L. Physical Review Letters, Vol. 111, Issue 2, Article No. 025901 https://doi.org/10.1103/PhysRevLett.111.025901	journal	July 2013
Three-Dimensional Imaging of Individual Dopant Atoms in SrTiO 3 Hwang, Jinwoo; Zhang, Jack Y.; D’Alfonso, Adrian J. Physical Review Letters, Vol. 111, Issue 26 https://doi.org/10.1103/PhysRevLett.111.266101	journal	December 2013
Quantitative STEM Imaging of Order-Disorder Phenomena in Double Perovskite Thin Films Esser, B. D.; Hauser, A. J.; Williams, R. E. A. Physical Review Letters, Vol. 117, Issue 17 https://doi.org/10.1103/PhysRevLett.117.176101	journal	October 2016
Exceptionally Strong Phonon Scattering by B Substitution in Cubic SiC Katre, Ankita; Carrete, Jesús; Dongre, Bonny Physical Review Letters, Vol. 119, Issue 7 https://doi.org/10.1103/PhysRevLett.119.075902	journal	August 2017
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
New group III-group V compounds: BP and BAs Perri, J. A.; La Placa, S.; Post, B. Acta Crystallographica, Vol. 11, Issue 4 https://doi.org/10.1107/S0365110X58000827	journal	April 1958
Experimental observation of high thermal conductivity in boron arsenide Kang, Joon Sang; Li, Man; Wu, Huan Science, Vol. 361, Issue 6402 https://doi.org/10.1126/science.aat5522	journal	July 2018
Unusual high thermal conductivity in boron arsenide bulk crystals Tian, Fei; Song, Bai; Chen, Xi Science, Vol. 361, Issue 6402 https://doi.org/10.1126/science.aat7932	journal	July 2018
High thermal conductivity in cubic boron arsenide crystals Li, Sheng; Zheng, Qiye; Lv, Yinchuan Science, Vol. 361, Issue 6402 https://doi.org/10.1126/science.aat8982	journal	July 2018
The B-Li (Boron-Lithium) system Borgstedt, H. B.; Guminski, C. Journal of Phase Equilibria, Vol. 24, Issue 6 https://doi.org/10.1361/105497103772084723	journal	December 2003
Exceptionally strong phonon scattering by B substitution in cubic SiC Katre, Ankita; Carrete, Jesús; Dongre, Bonny arXiv https://doi.org/10.48550/arxiv.1703.04996	text	January 2017
An ultrasensitive molybdenum-based double-heterojunction phototransistor Zenodo https://doi.org/10.5281/zenodo.4835973	text	January 2021

Cited By (6)

High Thermal Conductivity in Boron Arsenide: From Prediction to Reality Tian, Fei; Ren, Zhifeng Angewandte Chemie, Vol. 131, Issue 18 https://doi.org/10.1002/ange.201812112	journal	April 2019
High Thermal Conductivity in Boron Arsenide: From Prediction to Reality Tian, Fei; Ren, Zhifeng Angewandte Chemie International Edition, Vol. 58, Issue 18 https://doi.org/10.1002/anie.201812112	journal	April 2019
Impurity-derived p -type conductivity in cubic boron arsenide Lyons, John L.; Varley, Joel B.; Glaser, Evan R. Applied Physics Letters, Vol. 113, Issue 25 https://doi.org/10.1063/1.5058134	journal	December 2018
Point defects and dopants of boron arsenide from first-principles calculations: Donor compensation and doping asymmetry Chae, S.; Mengle, K.; Heron, J. T. Applied Physics Letters, Vol. 113, Issue 21 https://doi.org/10.1063/1.5062267	journal	November 2018
Perspective on ab initio phonon thermal transport Lindsay, Lucas; Katre, Ankita; Cepellotti, Andrea Journal of Applied Physics, Vol. 126, Issue 5 https://doi.org/10.1063/1.5108651	journal	August 2019
Electronic band structure and optical properties of boron arsenide Buckeridge, J.; Scanlon, D. O. Physical Review Materials, Vol. 3, Issue 5 https://doi.org/10.1103/physrevmaterials.3.051601	journal	May 2019