Spin-orbit coupling effects on predicting defect properties with hybrid functionals: A case study in CdTe
Abstract
Defect formation energies and transition levels are critical in determining doping behavior and recombination in semiconductor applications. Hybrid functionals are often used to overcome the band gap and delocalization errors of standard density-functional theory, and it is tempting to presume that the defect properties are correctly predicted once the hybrid functional mixing parameter reproduces the experimental band gap. However, pronounced spin-orbit coupling (SOC) effects can have an additional important role, which is clearly shown in this work by analyzing SOC effects originating from the Te-p orbitals in CdTe. In this work, we therefore use a hybrid functional that reproduces the experimental band gap when SOC is included, requiring a larger mixing parameter a=0.33 compared to the conventional choice of a=0.25. This hybrid functional was then used to predict defect properties, e.g., formation energy, transition level, and defect equilibrium. For defect states that do not directly involve the Te-p orbitals, such as the Cd interstitial (Cdi), we find that the effect of SOC on the defect levels can be captured by simply considering the SOC-induced band-edge shift. This is not the case for the A center (ClTe-VCd defect pair), where the localized acceptor state formed by Te-p orbitals is more directlymore »
- Authors:
-
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1475126
- Alternate Identifier(s):
- OSTI ID: 1465890
- Report Number(s):
- NREL/JA-5K00-72123
Journal ID: ISSN 2469-9950; PRBMDO
- Grant/Contract Number:
- AC36-08GO28308; DEAC36-08GO28308; EE0006344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 98; Journal Issue: 5; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; hybrid functionals; band gap; spin-orbit coupling; defect formation
Citation Formats
Pan, Jie, Metzger, Wyatt K., and Lany, Stephan. Spin-orbit coupling effects on predicting defect properties with hybrid functionals: A case study in CdTe. United States: N. p., 2018.
Web. doi:10.1103/PhysRevB.98.054108.
Pan, Jie, Metzger, Wyatt K., & Lany, Stephan. Spin-orbit coupling effects on predicting defect properties with hybrid functionals: A case study in CdTe. United States. https://doi.org/10.1103/PhysRevB.98.054108
Pan, Jie, Metzger, Wyatt K., and Lany, Stephan. Wed .
"Spin-orbit coupling effects on predicting defect properties with hybrid functionals: A case study in CdTe". United States. https://doi.org/10.1103/PhysRevB.98.054108. https://www.osti.gov/servlets/purl/1475126.
@article{osti_1475126,
title = {Spin-orbit coupling effects on predicting defect properties with hybrid functionals: A case study in CdTe},
author = {Pan, Jie and Metzger, Wyatt K. and Lany, Stephan},
abstractNote = {Defect formation energies and transition levels are critical in determining doping behavior and recombination in semiconductor applications. Hybrid functionals are often used to overcome the band gap and delocalization errors of standard density-functional theory, and it is tempting to presume that the defect properties are correctly predicted once the hybrid functional mixing parameter reproduces the experimental band gap. However, pronounced spin-orbit coupling (SOC) effects can have an additional important role, which is clearly shown in this work by analyzing SOC effects originating from the Te-p orbitals in CdTe. In this work, we therefore use a hybrid functional that reproduces the experimental band gap when SOC is included, requiring a larger mixing parameter a=0.33 compared to the conventional choice of a=0.25. This hybrid functional was then used to predict defect properties, e.g., formation energy, transition level, and defect equilibrium. For defect states that do not directly involve the Te-p orbitals, such as the Cd interstitial (Cdi), we find that the effect of SOC on the defect levels can be captured by simply considering the SOC-induced band-edge shift. This is not the case for the A center (ClTe-VCd defect pair), where the localized acceptor state formed by Te-p orbitals is more directly affected by the SOC. For this defect, a mixing parameter as large as a=0.40 is required to reproduce the experimental acceptor level. Regarding the implications for photovoltaics, we suggest that the Cdi, which is the dominant compensating donor, could play an important role as a recombination center. While Cdi is usually thought of as a benign shallow donor, our predicted defect levels in the fully band-gap-corrected calculations are deep enough to raise a concern, and we propose a recombination mechanism for electron capture by Cdi.},
doi = {10.1103/PhysRevB.98.054108},
journal = {Physical Review B},
number = 5,
volume = 98,
place = {United States},
year = {Wed Aug 22 00:00:00 EDT 2018},
month = {Wed Aug 22 00:00:00 EDT 2018}
}
Web of Science
Works referenced in this record:
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
CdCl 2 Treatment-Induced Enhanced Conductivity in CdTe Solar Cells Observed Using Conductive Atomic Force Microscopy
journal, November 2016
- Tuteja, Mohit; Mei, Antonio B.; Palekis, Vasilios
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 24
Non-Radiative Carrier Recombination Enhanced by Two-Level Process: A First-Principles Study
journal, February 2016
- Yang, Ji-Hui; Shi, Lin; Wang, Lin-Wang
- Scientific Reports, Vol. 6, Issue 1
Ab initio Calculations of Deep-Level Carrier Nonradiative Recombination Rates in Bulk Semiconductors
journal, December 2012
- Shi, Lin; Wang, Lin-Wang
- Physical Review Letters, Vol. 109, Issue 24
High temperature CSS processed CdTe solar cells on commercial SnO2:F/SnO2 coated soda-lime glass substrates
journal, March 2015
- Paudel, Naba R.; Grice, Corey R.; Xiao, Chuanxiao
- Journal of Materials Science: Materials in Electronics, Vol. 26, Issue 7
Statistics of the Recombinations of Holes and Electrons
journal, September 1952
- Shockley, W.; Read, W. T.
- Physical Review, Vol. 87, Issue 5
The roles of carrier concentration and interface, bulk, and grain-boundary recombination for 25% efficient CdTe solar cells
journal, June 2017
- Kanevce, A.; Reese, M. O.; Barnes, T. M.
- Journal of Applied Physics, Vol. 121, Issue 21
Measurement and Assessment of the Thermodynamic Properties and the Phase Diagram of the Cd–Te System
journal, January 2000
- Yamaguchi, K.; Hongo, K.; Hack, K.
- Materials Transactions, JIM, Vol. 41, Issue 7
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Electronic Correlation in Anion Orbitals Impedes Ferromagnetism due to Cation Vacancies in Zn Chalcogenides
journal, July 2009
- Chan, J. A.; Lany, Stephan; Zunger, Alex
- Physical Review Letters, Vol. 103, Issue 1
Density Functional Calculations of Native Defects in CH 3 NH 3 PbI 3 : Effects of Spin–Orbit Coupling and Self-Interaction Error
journal, April 2015
- Du, Mao-Hua
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 8
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998
- Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
- Physical Review B, Vol. 57, Issue 3, p. 1505-1509
Energy band gap, intrinsic carrier concentration, and Fermi level of CdTe bulk crystal between 304 and 1067K
journal, April 2008
- Su, Ching-Hua
- Journal of Applied Physics, Vol. 103, Issue 8
General method to predict voltage-dependent ionic conduction in a solid electrolyte coating on electrodes
journal, April 2015
- Pan, Jie; Cheng, Yang-Tse; Qi, Yue
- Physical Review B, Vol. 91, Issue 13
Theoretical Considerations Governing the Choice of the Optimum Semiconductor for Photovoltaic Solar Energy Conversion
journal, July 1956
- Loferski, Joseph J.
- Journal of Applied Physics, Vol. 27, Issue 7
Accurate prediction of defect properties in density functional supercell calculations
journal, November 2009
- Lany, Stephan; Zunger, Alex
- Modelling and Simulation in Materials Science and Engineering, Vol. 17, Issue 8
Excitonic Effects in Methylammonium Lead Halide Perovskites
journal, May 2018
- Chen, Xihan; Lu, Haipeng; Yang, Ye
- The Journal of Physical Chemistry Letters, Vol. 9, Issue 10
Assessment of correction methods for the band-gap problem and for finite-size effects in supercell defect calculations: Case studies for ZnO and GaAs
journal, December 2008
- Lany, Stephan; Zunger, Alex
- Physical Review B, Vol. 78, Issue 23, Article No. 235104
Polaronic hole localization and multiple hole binding of acceptors in oxide wide-gap semiconductors
journal, August 2009
- Lany, Stephan; Zunger, Alex
- Physical Review B, Vol. 80, Issue 8
Correcting density functional theory for accurate predictions of compound enthalpies of formation: Fitted elemental-phase reference energies
journal, March 2012
- Stevanović, Vladan; Lany, Stephan; Zhang, Xiuwen
- Physical Review B, Vol. 85, Issue 11
Predicting magnetism: Self-interaction correction scheme
journal, October 2008
- Droghetti, A.; Pemmaraju, C. D.; Sanvito, S.
- Physical Review B, Vol. 78, Issue 14
Semiconducting transition-metal oxides based on cations: Theory for MnO and Fe O
journal, May 2012
- Peng, Haowei; Lany, Stephan
- Physical Review B, Vol. 85, Issue 20
Strong spin-orbit splitting and magnetism of point defect states in monolayer
journal, November 2016
- Li, Wun-Fan; Fang, Changming; van Huis, Marijn A.
- Physical Review B, Vol. 94, Issue 19
Theoretical study of intrinsic defects in CdTe
journal, May 2016
- Menéndez-Proupin, E.; Orellana, W.
- Journal of Physics: Conference Series, Vol. 720
Native defects in second-generation topological insulators: Effect of spin-orbit interaction on Bi Se
journal, September 2012
- West, D.; Sun, Y. Y.; Wang, Han
- Physical Review B, Vol. 86, Issue 12
First-principles calculations for defects and impurities: Applications to III-nitrides
journal, April 2004
- Van de Walle, Chris G.; Neugebauer, Jörg
- Journal of Applied Physics, Vol. 95, Issue 8
CdS/CdTe thin-film solar cells with Cu-free transition metal oxide/Au back contacts: CdTe cells with Cu-free TMO/Au back contacts
journal, December 2013
- Paudel, Naba Raj; Xiao, Chuanxiao; Yan, Yanfa
- Progress in Photovoltaics: Research and Applications, Vol. 23, Issue 4
What causes high resistivity in CdTe
journal, June 2012
- Biswas, Koushik; Du, Mao-Hua
- New Journal of Physics, Vol. 14, Issue 6
Influence of the exchange screening parameter on the performance of screened hybrid functionals
journal, December 2006
- Krukau, Aliaksandr V.; Vydrov, Oleg A.; Izmaylov, Artur F.
- The Journal of Chemical Physics, Vol. 125, Issue 22
Non-radiative transitions in semiconductors
journal, December 1981
- Stoneham, A. M.
- Reports on Progress in Physics, Vol. 44, Issue 12
First-principles study of roles of Cu and Cl in polycrystalline CdTe
journal, January 2016
- Yang, Ji-Hui; Yin, Wan-Jian; Park, Ji-Sang
- Journal of Applied Physics, Vol. 119, Issue 4
Density functional theory description of hole-trapping in : A self-interaction-corrected approach
journal, May 2005
- d’Avezac, Mayeul; Calandra, Matteo; Mauri, Francesco
- Physical Review B, Vol. 71, Issue 20
High-efficiency polycrystalline CdTe thin-film solar cells
journal, December 2004
- Wu, Xuanzhi
- Solar Energy, Vol. 77, Issue 6
Obtaining Large Columnar CdTe Grains and Long Lifetime on Nanocrystalline CdSe, MgZnO, or CdS Layers
journal, January 2018
- Amarasinghe, Mahisha; Colegrove, Eric; Moseley, John
- Advanced Energy Materials, Vol. 8, Issue 11
Chemical potential dependence of defect formation energies in GaAs: Application to Ga self-diffusion
journal, October 1991
- Zhang, S.; Northrup, John
- Physical Review Letters, Vol. 67, Issue 17
Review on first-principles study of defect properties of CdTe as a solar cell absorber
journal, July 2016
- Yang, Ji-Hui; Yin, Wan-Jian; Park, Ji-Sang
- Semiconductor Science and Technology, Vol. 31, Issue 8
Identification of the chlorine A center in CdTe
journal, March 1992
- Hofmann, D. M.; Omling, P.; Grimmeiss, H. G.
- Physical Review B, Vol. 45, Issue 11
First-principles calculations for point defects in solids
journal, March 2014
- Freysoldt, Christoph; Grabowski, Blazej; Hickel, Tilmann
- Reviews of Modern Physics, Vol. 86, Issue 1
The Perdew–Burke–Ernzerhof exchange-correlation functional applied to the G2-1 test set using a plane-wave basis set
journal, June 2005
- Paier, Joachim; Hirschl, Robin; Marsman, Martijn
- The Journal of Chemical Physics, Vol. 122, Issue 23
Semiconductor Charge Densities with Hard-Core and Soft-Core Pseudopotentials
journal, March 1979
- Hamann, D. R.
- Physical Review Letters, Vol. 42, Issue 10
Defect interactions and the role of complexes in the CdTe solar cell absorber
journal, January 2017
- Krasikov, Dmitry; Sankin, Igor
- Journal of Materials Chemistry A, Vol. 5, Issue 7
Overcoming the doping bottleneck in semiconductors
journal, August 2004
- Wei, Su-Huai
- Computational Materials Science, Vol. 30, Issue 3-4
First-principles theory of nonradiative carrier capture via multiphonon emission
journal, August 2014
- Alkauskas, Audrius; Yan, Qimin; Van de Walle, Chris G.
- Physical Review B, Vol. 90, Issue 7
Defect Energy Levels in Density Functional Calculations: Alignment and Band Gap Problem
journal, July 2008
- Alkauskas, Audrius; Broqvist, Peter; Pasquarello, Alfredo
- Physical Review Letters, Vol. 101, Issue 4
Direct Observation of CdCl 2 Treatment Induced Grain Boundary Carrier Depletion in CdTe Solar Cells Using Scanning Probe Microwave Reflectivity Based Capacitance Measurements
journal, March 2016
- Tuteja, Mohit; Koirala, Prakash; Palekis, Vasilios
- The Journal of Physical Chemistry C, Vol. 120, Issue 13
Calculation of the magnetic anisotropy with projected-augmented-wave methodology and the case study of disordered alloys
journal, June 2016
- Steiner, Soner; Khmelevskyi, Sergii; Marsmann, Martijn
- Physical Review B, Vol. 93, Issue 22
Electrically active point defects in cadmium telluride
journal, March 1970
- Smith, F. T. J.
- Metallurgical and Materials Transactions B, Vol. 1, Issue 3
Effect of spin-orbit coupling on formation of native defects in Weyl fermion semimetals: The case of ;
journal, November 2016
- Yu, Zhi Gen; Zhang, Yong-Wei
- Physical Review B, Vol. 94, Issue 19
Electron-Hole Recombination in Germanium
journal, July 1952
- Hall, R. N.
- Physical Review, Vol. 87, Issue 2
Tuning the Fermi level beyond the equilibrium doping limit through quenching: The case of CdTe
journal, December 2014
- Yang, Ji-Hui; Park, Ji-Sang; Kang, Joongoo
- Physical Review B, Vol. 90, Issue 24
Works referencing / citing this record:
Interplay between Composition, Electronic Structure, Disorder, and Doping due to Dual Sublattice Mixing in Nonequilibrium Synthesis of ZnSnN 2 :O
journal, January 2019
- Pan, Jie; Cordell, Jacob; Tucker, Garritt J.
- Advanced Materials, Vol. 31, Issue 11
Radiative Efficiency and Charge‐Carrier Lifetimes and Diffusion Length in Polycrystalline CdSeTe Heterostructures
journal, December 2019
- Kuciauskas, Darius; Moseley, John; Ščajev, Patrik
- physica status solidi (RRL) – Rapid Research Letters, Vol. 14, Issue 3
Machine-learned impurity level prediction for semiconductors: the example of Cd-based chalcogenides
journal, April 2020
- Mannodi-Kanakkithodi, Arun; Toriyama, Michael Y.; Sen, Fatih G.
- npj Computational Materials, Vol. 6, Issue 1
Self-compensation in chlorine-doped CdTe
journal, June 2019
- Orellana, Walter; Menéndez-Proupin, Eduardo; Flores, Mauricio A.
- Scientific Reports, Vol. 9, Issue 1
Electron scattering mechanisms in polycrystalline sputtered zinc tin oxynitride thin films
journal, July 2019
- Hamilton, Dylan C.; Arca, Elisabetta; Pan, Jie
- Journal of Applied Physics, Vol. 126, Issue 3
Enhancement of photovoltaic efficiency in CdSe x Te 1− x (where 0 ⩽ x ⩽ 1): insights from density functional theory
journal, December 2019
- Watts, Michael J.; Fiducia, Thomas A. M.; Sanyal, Biplab
- Journal of Physics: Condensed Matter, Vol. 32, Issue 12
Radiative Efficiency and Charge‐Carrier Lifetimes and Diffusion Length in Polycrystalline CdSeTe Heterostructures
journal, January 2020
- Kuciauskas, Darius; Moseley, John; Ščajev, Patrik
- physica status solidi (RRL) – Rapid Research Letters, Vol. 14, Issue 3