Ab initio study of intrinsic point defects in PbTe: an insight into phase stability
Abstract
The stability of intrinsic point defects in PbTe, one of the most widely studied and efficient thermoelectric material, is explored by means of Density Functional Theory (DFT). The origin of n- and p-type conductivity in PbTe is attributed to particular intrinsic charged defects by calculating their formation energies. Here, these DFT calculated defect formation energies are then used in the Gibbs free energy description of this phase as part of the Pb-Te thermodynamic model built using the CALPHAD method, and in the resulting phase diagram it is found that its solubility lines and non-stoichiometric range agree very well with experimental data. Such an approach of using DFT in conjunction with CALPHAD for compound semiconductor phases that exhibit very small ranges of non-stoichiometry does not only make the process of calculating phase diagrams for such systems more physical, but is necessary and critical for the assessment of unknown phase diagrams.
- Authors:
-
- California Inst. of Technology (CalTech), Pasadena, CA (United States)
- Northwestern Univ., Evanston, IL (United States)
- National Dong Hwa Univ. (Taiwan)
- National Sun Yat-sen Univ., Kaohsiung (Taiwan)
- National Tsing Hua Univ., Hsin-Chu (Taiwan)
- California Inst. of Technology (CalTech), Pasadena, CA (United States); Northwestern Univ., Evanston, IL (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Revolutionary Materials for Solid State Energy Conversion (RMSSEC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Council of Taiwan
- OSTI Identifier:
- 1370315
- Alternate Identifier(s):
- OSTI ID: 1251475
- Grant/Contract Number:
- SC0001054; W31P4Q-13-1-0010; AC02-05CH11231; NSC101-3113-P-008-001
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Acta Materialia
- Additional Journal Information:
- Journal Volume: 92; Related Information: RMSSEC partners with Michigan State University (lead); University of California, Los Angeles; University of Michigan; Northwestern University; Oak Ridge National Laboratory; Ohio State University; Wayne State University; Journal ID: ISSN 1359-6454
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Point defects; Thermoelectric; DFT; CALPHAD
Citation Formats
Bajaj, Saurabh, Pomrehn, Gregory S., Doak, Jeff W., Gierlotka, Wojciech, Wu, Hsin-jay, Chen, Sinn-Wen, Wolverton, Chris, Goddard, III, William A., and Snyder, G. Jeffrey. Ab initio study of intrinsic point defects in PbTe: an insight into phase stability. United States: N. p., 2015.
Web. doi:10.1016/j.actamat.2015.03.034.
Bajaj, Saurabh, Pomrehn, Gregory S., Doak, Jeff W., Gierlotka, Wojciech, Wu, Hsin-jay, Chen, Sinn-Wen, Wolverton, Chris, Goddard, III, William A., & Snyder, G. Jeffrey. Ab initio study of intrinsic point defects in PbTe: an insight into phase stability. United States. https://doi.org/10.1016/j.actamat.2015.03.034
Bajaj, Saurabh, Pomrehn, Gregory S., Doak, Jeff W., Gierlotka, Wojciech, Wu, Hsin-jay, Chen, Sinn-Wen, Wolverton, Chris, Goddard, III, William A., and Snyder, G. Jeffrey. 2015.
"Ab initio study of intrinsic point defects in PbTe: an insight into phase stability". United States. https://doi.org/10.1016/j.actamat.2015.03.034. https://www.osti.gov/servlets/purl/1370315.
@article{osti_1370315,
title = {Ab initio study of intrinsic point defects in PbTe: an insight into phase stability},
author = {Bajaj, Saurabh and Pomrehn, Gregory S. and Doak, Jeff W. and Gierlotka, Wojciech and Wu, Hsin-jay and Chen, Sinn-Wen and Wolverton, Chris and Goddard, III, William A. and Snyder, G. Jeffrey},
abstractNote = {The stability of intrinsic point defects in PbTe, one of the most widely studied and efficient thermoelectric material, is explored by means of Density Functional Theory (DFT). The origin of n- and p-type conductivity in PbTe is attributed to particular intrinsic charged defects by calculating their formation energies. Here, these DFT calculated defect formation energies are then used in the Gibbs free energy description of this phase as part of the Pb-Te thermodynamic model built using the CALPHAD method, and in the resulting phase diagram it is found that its solubility lines and non-stoichiometric range agree very well with experimental data. Such an approach of using DFT in conjunction with CALPHAD for compound semiconductor phases that exhibit very small ranges of non-stoichiometry does not only make the process of calculating phase diagrams for such systems more physical, but is necessary and critical for the assessment of unknown phase diagrams.},
doi = {10.1016/j.actamat.2015.03.034},
url = {https://www.osti.gov/biblio/1370315},
journal = {Acta Materialia},
issn = {1359-6454},
number = ,
volume = 92,
place = {United States},
year = {Mon Apr 13 00:00:00 EDT 2015},
month = {Mon Apr 13 00:00:00 EDT 2015}
}
Web of Science
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