First-principles calculation of intrinsic defect chemistry and self-doping in PbTe

Goyal, Anuj; Gorai, Prashun; Toberer, Eric S.; Stevanovic, Vladan

doi:10.1038/s41524-017-0047-6

Title: First-principles calculation of intrinsic defect chemistry and self-doping in PbTe

Journal Article · Fri Nov 10 00:00:00 EST 2017 · npj Computational Materials

DOI:https://doi.org/10.1038/s41524-017-0047-6· OSTI ID:1432441

Goyal, Anuj ^[1]; Gorai, Prashun ^[1]; Toberer, Eric S. ^[1]; Stevanovic, Vladan ^[1]

Colorado School of Mines, Golden, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)

Semiconductor dopability is inherently limited by intrinsic defect chemistry. In many thermoelectric materials, narrow band gaps due to strong spin-orbit interactions make accurate atomic level predictions of intrinsic defect chemistry and self-doping computationally challenging. For this study, we use different levels of theory to model point defects in PbTe, and compare and contrast the results against each other and a large body of experimental data. We find that to accurately reproduce the intrinsic defect chemistry and known self-doping behavior of PbTe, it is essential to (a) go beyond the semi-local GGA approximation to density functional theory, (b) include spin-orbit coupling, and (c) utilize many-body GW theory to describe the positions of individual band edges. The hybrid HSE functional with spin-orbit coupling included, in combination with the band edge shifts from G0W0 is the only approach that accurately captures both the intrinsic conductivity type of PbTe as function of synthesis conditions as well as the measured charge carrier concentrations, without the need for experimental inputs. Our results reaffirm the critical role of the position of individual band edges in defect calculations, and demonstrate that dopability can be accurately predicted in such challenging narrow band gap materials.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)

Grant/Contract Number:: AC36-08GO28308; DMR-1309980; 1334713

OSTI ID:: 1432441

Report Number(s):: NREL/JA-5K00-71271

Journal Information:: npj Computational Materials, Vol. 3, Issue 1; ISSN 2057-3960

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 57 works

Citation information provided by
Web of Science

References (52)

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
Thermoelectric Performance and Defect Chemistry in n-Type Zintl KGaSb ₄ Ortiz, Brenden R.; Gorai, Prashun; Stevanović, Vladan Chemistry of Materials, Vol. 29, Issue 10 https://doi.org/10.1021/acs.chemmater.7b01217	journal	May 2017
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
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
Practical doping principles Zunger, Alex Applied Physics Letters, Vol. 83, Issue 1 https://doi.org/10.1063/1.1584074	journal	July 2003
Complex thermoelectric materials Snyder, G. Jeffrey; Toberer, Eric S. Nature Materials, Vol. 7, Issue 2, p. 105-114 https://doi.org/10.1038/nmat2090	journal	February 2008
Theoretical study of deep-defect states in bulk PbTe and in thin films Hoang, Khang; Mahanti, S. D.; Jena, Puru Physical Review B, Vol. 76, Issue 11 https://doi.org/10.1103/PhysRevB.76.115432	journal	September 2007
Composition Limits of Stability of PbTe Brebrick, R. F.; Allgaier, R. S. The Journal of Chemical Physics, Vol. 32, Issue 6 https://doi.org/10.1063/1.1731029	journal	June 1960
Unraveling the Native Conduction of Trichalcogenides and Its Ideal Band Alignment for New Photovoltaic Interfaces Tumelero, Milton A.; Faccio, Ricardo; Pasa, Andre A. The Journal of Physical Chemistry C, Vol. 120, Issue 3 https://doi.org/10.1021/acs.jpcc.5b10233	journal	January 2016
Ab initio studies of the electronic structure of defects in PbTe Ahmad, Salameh; Mahanti, S. D.; Hoang, Khang Physical Review B, Vol. 74, Issue 15 https://doi.org/10.1103/PhysRevB.74.155205	journal	October 2006
Accurate prediction of defect properties in density functional supercell calculations Lany, Stephan; Zunger, Alex Modelling and Simulation in Materials Science and Engineering, Vol. 17, Issue 8 https://doi.org/10.1088/0965-0393/17/8/084002	journal	November 2009
The high-throughput highway to computational materials design Curtarolo, Stefano; Hart, Gus L. W.; Nardelli, Marco Buongiorno Nature Materials, Vol. 12, Issue 3 https://doi.org/10.1038/nmat3568	journal	February 2013
Hydrogen as a Cause of Doping in Zinc Oxide Van de Walle, Chris G. Physical Review Letters, Vol. 85, Issue 5 https://doi.org/10.1103/PhysRevLett.85.1012	journal	July 2000
Computationally guided discovery of thermoelectric materials Gorai, Prashun; Stevanović, Vladan; Toberer, Eric S. Nature Reviews Materials, Vol. 2, Issue 9 https://doi.org/10.1038/natrevmats.2017.53	journal	August 2017
A new mixing of Hartree–Fock and local density‐functional theories Becke, Axel D. The Journal of Chemical Physics, Vol. 98, Issue 2 https://doi.org/10.1063/1.464304	journal	January 1993
High thermoelectric figure of merit in heavy hole dominated PbTe Pei, Yanzhong; LaLonde, Aaron; Iwanaga, Shiho Energy & Environmental Science, Vol. 4, Issue 6 https://doi.org/10.1039/c0ee00456a	journal	January 2011
Electronic and structural anomalies in lead chalcogenides Wei, Su-Huai; Zunger, Alex Physical Review B, Vol. 55, Issue 20 https://doi.org/10.1103/PhysRevB.55.13605	journal	May 1997
Nonstoichiometry and point defects in PbTe Schenk, M.; Berger, H.; Klimakow, A. Crystal Research and Technology, Vol. 23, Issue 1 https://doi.org/10.1002/crat.2170230111	journal	January 1988
Dopability, Intrinsic Conductivity, and Nonstoichiometry of Transparent Conducting Oxides Lany, Stephan; Zunger, Alex Physical Review Letters, Vol. 98, Issue 4 https://doi.org/10.1103/PhysRevLett.98.045501	journal	January 2007
Correcting density functional theory for accurate predictions of compound enthalpies of formation: Fitted elemental-phase reference energies Stevanović, Vladan; Lany, Stephan; Zhang, Xiuwen Physical Review B, Vol. 85, Issue 11 https://doi.org/10.1103/PhysRevB.85.115104	journal	March 2012
Electrical and Optical Properties of Epitaxial Films of PbS, PbSe, PbTe, and SnTe Zemel, Jay N.; Jensen, James D.; Schoolar, Richard B. Physical Review, Vol. 140, Issue 1A https://doi.org/10.1103/PhysRev.140.A330	journal	October 1965
Theoretical and experimental investigations of the thermoelectric properties of Bi ₂ S ₃ Chmielowski, Radoslaw; Péré, Daniel; Bera, Chandan Journal of Applied Physics, Vol. 117, Issue 12 https://doi.org/10.1063/1.4916528	journal	March 2015
Electronic structure calculations of lead chalcogenides PbS, PbSe, PbTe Lach-hab, Mohammed; Papaconstantopoulos, Dimitrios A.; Mehl, Michael J. Journal of Physics and Chemistry of Solids, Vol. 63, Issue 5 https://doi.org/10.1016/S0022-3697(01)00237-2	journal	May 2002
Composition Stability Limits of PbTe. II Brebrick, R. F.; Gubner, E. The Journal of Chemical Physics, Vol. 36, Issue 5 https://doi.org/10.1063/1.1732728	journal	March 1962
Index matching far-infrared method for measuring the static dielectric constant of PbTe Tennant, W. E. Solid State Communications, Vol. 20, Issue 6 https://doi.org/10.1016/0038-1098(76)91072-3	journal	November 1976
Thermal physics of the lead chalcogenides PbS, PbSe, and PbTe from first principles Skelton, Jonathan M.; Parker, Stephen C.; Togo, Atsushi Physical Review B, Vol. 89, Issue 20 https://doi.org/10.1103/PhysRevB.89.205203	journal	May 2014
A computational framework for automation of point defect calculations Goyal, Anuj; Gorai, Prashun; Peng, Haowei Computational Materials Science, Vol. 130 https://doi.org/10.1016/j.commatsci.2016.12.040	journal	April 2017
Native defects in second-generation topological insulators: Effect of spin-orbit interaction on Bi $_{2}$ Se $_{3}$ West, D.; Sun, Y. Y.; Wang, Han Physical Review B, Vol. 86, Issue 12 https://doi.org/10.1103/PhysRevB.86.121201	journal	September 2012
First-principles calculations for defects and impurities: Applications to III-nitrides Van de Walle, Chris G.; Neugebauer, Jörg Journal of Applied Physics, Vol. 95, Issue 8 https://doi.org/10.1063/1.1682673	journal	April 2004
Surface morphology and ionization potentials of polar semiconductors: The case of GaAs Sgiarovello, C.; Binggeli, N.; Baldereschi, A. Physical Review B, Vol. 69, Issue 3 https://doi.org/10.1103/PhysRevB.69.035320	journal	January 2004
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
Structural and electronic properties of lead chalcogenides from first principles Hummer, Kerstin; Grüneis, Andreas; Kresse, Georg Physical Review B, Vol. 75, Issue 19 https://doi.org/10.1103/PhysRevB.75.195211	journal	May 2007
Band-edge problem in the theoretical determination of defect energy levels: The O vacancy in ZnO as a benchmark case Alkauskas, Audrius; Pasquarello, Alfredo Physical Review B, Vol. 84, Issue 12 https://doi.org/10.1103/PhysRevB.84.125206	journal	September 2011
Annealing studies of PbTe and Pb _{1− x} Sn _x Te Hewes, C. Robert; Adler, Michael S.; Senturia, Stephen D. Journal of Applied Physics, Vol. 44, Issue 3 https://doi.org/10.1063/1.1662348	journal	March 1973
Electron and chemical reservoir corrections for point-defect formation energies Freysoldt, Christoph; Lange, Björn; Neugebauer, Jörg Physical Review B, Vol. 93, Issue 16 https://doi.org/10.1103/PhysRevB.93.165206	journal	April 2016
Electronic structure, structural properties, and dielectric functions of IV-VI semiconductors: PbSe and PbTe Albanesi, E. A.; Okoye, C. M. I.; Rodriguez, C. O. Physical Review B, Vol. 61, Issue 24 https://doi.org/10.1103/PhysRevB.61.16589	journal	June 2000
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
New Method for Calculating the One-Particle Green's Function with Application to the Electron-Gas Problem Hedin, Lars Physical Review, Vol. 139, Issue 3A https://doi.org/10.1103/PhysRev.139.A796	journal	August 1965
Calculation of the Temperature Dependence of the Energy Gaps in PbTe and SnTe Tsang, Y. W.; Cohen, Marvin L. Physical Review B, Vol. 3, Issue 4 https://doi.org/10.1103/PhysRevB.3.1254	journal	February 1971
Ab initio calculation of the macroscopic dielectric constant in silicon Baroni, Stefano; Resta, Raffaele Physical Review B, Vol. 33, Issue 10 https://doi.org/10.1103/PhysRevB.33.7017	journal	May 1986
P - T - x Phase Diagram of the Lead Telluride System Fujimoto, Masatomo; Sato, Yasuo Japanese Journal of Applied Physics, Vol. 5, Issue 2 https://doi.org/10.1143/JJAP.5.128	journal	February 1966
Thermal and Optical Energy Gaps in PbTe Tauber, R. N.; Machonis, A. A.; Cadoff, I. B. Journal of Applied Physics, Vol. 37, Issue 13 https://doi.org/10.1063/1.1708150	journal	December 1966
First-principles calculations for point defects in solids Freysoldt, Christoph; Grabowski, Blazej; Hickel, Tilmann Reviews of Modern Physics, Vol. 86, Issue 1 https://doi.org/10.1103/RevModPhys.86.253	journal	March 2014
Linear optical properties in the projector-augmented wave methodology Gajdoš, M.; Hummer, K.; Kresse, G. Physical Review B, Vol. 73, Issue 4 https://doi.org/10.1103/PhysRevB.73.045112	journal	January 2006
Computational and experimental investigation of TmAgTe ₂ and XYZ ₂ compounds, a new group of thermoelectric materials identified by first-principles high-throughput screening Zhu, Hong; Hautier, Geoffroy; Aydemir, Umut Journal of Materials Chemistry C, Vol. 3, Issue 40 https://doi.org/10.1039/C5TC01440A	journal	January 2015
TE Design Lab: A virtual laboratory for thermoelectric material design Gorai, Prashun; Gao, Duanfeng; Ortiz, Brenden Computational Materials Science, Vol. 112 https://doi.org/10.1016/j.commatsci.2015.11.006	journal	February 2016
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
Photoemission Investigation of the Band Structure of PbTe Spicer, W. E.; Lapeyre, G. J. Physical Review, Vol. 139, Issue 2A https://doi.org/10.1103/PhysRev.139.A565	journal	July 1965
Quasiparticle self-consistent GW calculations for PbS, PbSe, and PbTe: Band structure and pressure coefficients Svane, A.; Christensen, N. E.; Cardona, M. Physical Review B, Vol. 81, Issue 24 https://doi.org/10.1103/PhysRevB.81.245120	journal	June 2010
Universal alignment of hydrogen levels in semiconductors, insulators and solutions Van de Walle, Chris G.; Neugebauer, J. Nature, Vol. 423, Issue 6940 https://doi.org/10.1038/nature01665	journal	June 2003
Ab initio study of intrinsic point defects in PbTe: an insight into phase stability Bajaj, Saurabh; Pomrehn, Gregory S.; Doak, Jeff W. Acta Materialia, Vol. 92 https://doi.org/10.1016/j.actamat.2015.03.034	journal	June 2015
High throughput density functional investigations of the stability, electronic structure and thermoelectric properties of binary silicides Opahle, Ingo; Madsen, Georg K. H.; Drautz, Ralf Physical Chemistry Chemical Physics, Vol. 14, Issue 47 https://doi.org/10.1039/c2cp41826f	journal	January 2012

Cited By (10)

Structural, Electronic and Thermoelectric Properties of Pb1−xSnxTe Alloys Pandit, Abhiyan; Haleoot, Raad; Hamad, Bothina Journal of Electronic Materials, Vol. 49, Issue 1 https://doi.org/10.1007/s11664-019-07715-4	journal	October 2019
The importance of phase equilibrium for doping efficiency: iodine doped PbTe Male, James; Agne, Matthias T.; Goyal, Anuj Materials Horizons, Vol. 6, Issue 7 https://doi.org/10.1039/c9mh00294d	journal	January 2019
A practical field guide to thermoelectrics: Fundamentals, synthesis, and characterization Zevalkink, Alex; Smiadak, David M.; Blackburn, Jeff L. Applied Physics Reviews, Vol. 5, Issue 2 https://doi.org/10.1063/1.5021094	journal	June 2018
Effective n-type doping of Mg3Sb2 with group-3 elements Gorai, Prashun; Toberer, Eric S.; Stevanović, Vladan Journal of Applied Physics, Vol. 125, Issue 2 https://doi.org/10.1063/1.5081833	journal	January 2019
Point defects in PbCdTe solid solutions Horichok, I. V.; Parashchuk, T. O. Journal of Applied Physics, Vol. 127, Issue 5 https://doi.org/10.1063/1.5130747	journal	February 2020
Ab initio modeling and design of vanadia-based electrode materials for post-lithium batteries Koch, Daniel; Manzhos, Sergei Journal of Physics D: Applied Physics, Vol. 53, Issue 8 https://doi.org/10.1088/1361-6463/ab4ca0	journal	December 2019
Effect of intrinsic defects on the thermal conductivity of PbTe from classical molecular dynamics simulations Troncoso, Javier F.; Aguado-Puente, Pablo; Kohanoff, Jorge Journal of Physics: Condensed Matter, Vol. 32, Issue 4 https://doi.org/10.1088/1361-648x/ab4aa8	journal	October 2019
Versatile electrical behavior of $1 T − {TiS}_{2}$ elucidated from a theoretical study Stoliaroff, Adrien; Latouche, Camille; Jobic, Stéphane Physical Review B, Vol. 99, Issue 16 https://doi.org/10.1103/physrevb.99.165122	journal	April 2019
Effective n-type Doping of Mg3Sb2 with Group-3 Elements Gorai, Prashun; Toberer, Eric S.; Stevanovic, Vladan Unpublished https://doi.org/10.13140/rg.2.2.19496.62720	text	January 2018
Metastable rocksalt ZnO is $p$-type dopable Goyal, Anuj; Stevanović, Vladan arXiv https://doi.org/10.48550/arxiv.1802.00360	text	January 2018

Similar Records

Ab initio study of point defects in PbSe and PbTe: Bulk and nanowire

Journal Article · Fri Nov 14 00:00:00 EST 2014 · Journal of Applied Physics · OSTI ID:1432441

Wrasse, E. O.; Venezuela, P.

The importance of phase equilibrium for doping efficiency: iodine doped PbTe

Journal Article · Wed Apr 03 00:00:00 EDT 2019 · Materials Horizons · OSTI ID:1432441

Male, James; Agne, Matthias T.; Goyal, Anuj; +4 more

Controlling thermoelectric transport via native defects in the diamond-like semiconductors Cu₂HgGeTe₄ and Hg₂GeTe₄

Journal Article · Fri Nov 05 00:00:00 EDT 2021 · Journal of Materials Chemistry. A · OSTI ID:1432441

Qu, Jiaxing; Porter, Claire E.; Gomes, Lídia C.; +5 more

Related Subjects

71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE
electronic structure
semiconductors
thermoelectrics

Title: First-principles calculation of intrinsic defect chemistry and self-doping in PbTe

Citation Formats

References (52)

Cited By (10)

Similar Records

Related Subjects