skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: 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:
 [1];  [1];  [2];  [3];  [4];  [5];  [2];  [1];  [6]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. National Dong Hwa Univ. (Taiwan)
  4. National Sun Yat-sen Univ., Kaohsiung (Taiwan)
  5. National Tsing Hua Univ., Hsin-Chu (Taiwan)
  6. 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}
}

Journal Article:

Citation Metrics:
Cited by: 42 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Complex thermoelectric materials
journal, February 2008


Composition Limits of Stability of PbTe
journal, June 1960


Annealing studies of PbTe and Pb 1− x Sn x Te
journal, March 1973


Precipitation of Te and Pb in PbTe Crystals
journal, April 1962


Ab initio studies of the electronic structure of defects in PbTe
journal, October 2006


Thermodynamic description of the Pb–Te system using ionic liquid model
journal, June 2009


Accurate prediction of defect properties in density functional supercell calculations
journal, November 2009


Periodic boundary conditions in ab initio calculations
journal, February 1995


Linear optical properties in the projector-augmented wave methodology
journal, January 2006


Ab initio calculation of the macroscopic dielectric constant in silicon
journal, May 1986


Ab initiomolecular dynamics for liquid metals
journal, January 1993


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Projector augmented-wave method
journal, December 1994


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Implementation of the projector augmented-wave LDA+U method: Application to the electronic structure of NiO
journal, December 2000


Generalized Gradient Approximation Made Simple
journal, October 1996


Special points for Brillouin-zone integrations
journal, June 1976


Thermodynamic Description of the Ag-Pb-Te Ternary System
journal, October 2010


SGTE data for pure elements
journal, October 1991


Optimization and calculation of the PB — TE system
journal, April 1986


The resistivity and thermoelectric power of liquid alloys containing tellurium
journal, March 1974


PbTe/CdTe single quantum wells grown on GaAs (100) substrates by molecular beam epitaxy
journal, September 2003


Thermodynamic Properties of Solid Monoxides, Monosulfides, Monoselenides, and Monotellurides of Ge, Sn, and Pb.
journal, January 1964


First-principles calculations for point defects in solids
journal, March 2014


Nonstoichiometry and point defects in PbTe
journal, January 1988


Thermo-Calc & DICTRA, computational tools for materials science
journal, June 2002


The U–Ti system: Strengths and weaknesses of the CALPHAD method
journal, December 2011


Die Mischungsenthalpien im System PbTe
journal, August 1983


Partial Pressures in Equilibrium with Group IV Tellurides. I. Optical Absorption Method and Results for PbTe
journal, June 1964


Works referencing / citing this record:

Fingerprints of native defects in monolayer PbTe
journal, January 2019


Effect of intrinsic defects on the thermal conductivity of PbTe from classical molecular dynamics simulations
journal, October 2019


Using First-Principles Calculations in CALPHAD Models to Determine Carrier Concentration of the Binary PbSe Semiconductor
journal, December 2018


Nb-Implanted BaO as a Support for Gold Single Atoms
journal, December 2021


Unveiling a Novel, Cation-Rich Compound in a High-Pressure Pb–Te Binary System
journal, April 2019


Prediction of Site Preference of Implanted Transition Metal Dopants in Rock-salt Oxides
journal, August 2019


On the origin of precipitation of transition metals implanted in MgO
journal, March 2021