Quasiparticle and hybrid density functional methods in defect studies: An application to the nitrogen vacancy in GaN
Abstract
Defects in semiconductors can play a vital role in the performance of electronic devices, with native defects often dominating the electronic properties of the semiconductor. Understanding the relationship between structural defects and electronic function will be central to the design of new high-performance materials. In particular, it is necessary to quantitatively understand the energy and lifetime of electronic states associated with the defect. In this work, we apply first-principles density functional theory (DFT) and many-body perturbation theory within the GW approximation to understand the nature and energy of the defect states associated with a charged nitrogen vacancy on the electronic properties of gallium nitride (GaN), as a model of a well-studied and important wide gap semiconductor grown with defects. We systematically investigate the sources of error associated with the GW approximation and the role of the underlying atomic structure on the predicted defect state energies. Additionally, analysis of the computed electronic density of states (DOS) reveals that there is one occupied defect state 0.2 eV below the valence band maximum and three unoccupied defect states at energy of 0.2–0.4 eV above the conduction band minimum, suggesting that this defect in the +1 charge state will not behave as a carriermore »
- Authors:
-
- Boston Univ., MA (United States). Dept. of Electrical and Computer Engineering
- Boston Univ., MA (United States). Dept. of Electrical and Computer Engineering and Dept. of Materials Science and Engineering
- Boston Univ., MA (United States). Dept. of Electrical and Computer Engineering, Dept. of Materials Science and Engineering and Dept. of Physics
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Science (SC); US Army Research Laboratory (USARL); National Science Foundation (NSF)
- OSTI Identifier:
- 1544347
- Alternate Identifier(s):
- OSTI ID: 1413819
- Grant/Contract Number:
- AC02-05CH11231; W911NF-12–2-0023; ACI-1548562
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 96; Journal Issue: 23; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Lewis, D. K., Matsubara, M., Bellotti, E., and Sharifzadeh, S. Quasiparticle and hybrid density functional methods in defect studies: An application to the nitrogen vacancy in GaN. United States: N. p., 2017.
Web. doi:10.1103/PhysRevB.96.235203.
Lewis, D. K., Matsubara, M., Bellotti, E., & Sharifzadeh, S. Quasiparticle and hybrid density functional methods in defect studies: An application to the nitrogen vacancy in GaN. United States. https://doi.org/10.1103/PhysRevB.96.235203
Lewis, D. K., Matsubara, M., Bellotti, E., and Sharifzadeh, S. Mon .
"Quasiparticle and hybrid density functional methods in defect studies: An application to the nitrogen vacancy in GaN". United States. https://doi.org/10.1103/PhysRevB.96.235203. https://www.osti.gov/servlets/purl/1544347.
@article{osti_1544347,
title = {Quasiparticle and hybrid density functional methods in defect studies: An application to the nitrogen vacancy in GaN},
author = {Lewis, D. K. and Matsubara, M. and Bellotti, E. and Sharifzadeh, S.},
abstractNote = {Defects in semiconductors can play a vital role in the performance of electronic devices, with native defects often dominating the electronic properties of the semiconductor. Understanding the relationship between structural defects and electronic function will be central to the design of new high-performance materials. In particular, it is necessary to quantitatively understand the energy and lifetime of electronic states associated with the defect. In this work, we apply first-principles density functional theory (DFT) and many-body perturbation theory within the GW approximation to understand the nature and energy of the defect states associated with a charged nitrogen vacancy on the electronic properties of gallium nitride (GaN), as a model of a well-studied and important wide gap semiconductor grown with defects. We systematically investigate the sources of error associated with the GW approximation and the role of the underlying atomic structure on the predicted defect state energies. Additionally, analysis of the computed electronic density of states (DOS) reveals that there is one occupied defect state 0.2 eV below the valence band maximum and three unoccupied defect states at energy of 0.2–0.4 eV above the conduction band minimum, suggesting that this defect in the +1 charge state will not behave as a carrier trap. Furthermore, we compare the character and energy of the defect state obtained from GW and DFT using the HSE approximate density functional and find excellent agreement. This systematic study provides a more complete understanding of how to obtain quantitative defect energy states in bulk semiconductors.},
doi = {10.1103/PhysRevB.96.235203},
journal = {Physical Review B},
number = 23,
volume = 96,
place = {United States},
year = {Mon Dec 18 00:00:00 EST 2017},
month = {Mon Dec 18 00:00:00 EST 2017}
}
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
Unraveling the Jahn-Teller effect in Mn-doped GaN using the Heyd-Scuseria-Ernzerhof hybrid functional
journal, May 2009
- Stroppa, A.; Kresse, G.
- Physical Review B, Vol. 79, Issue 20
Insights and challenges of applying the GW method to transition metal oxides
journal, October 2014
- Samsonidze, Georgy; Park, Cheol-Hwan; Kozinsky, Boris
- Journal of Physics: Condensed Matter, Vol. 26, Issue 47
Methodological aspects of the GW calculation of the carbon vacancy in 3C-SiC
journal, April 2012
- Bruneval, Fabien
- Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 277
Ab initio study of oxygen point defects in GaAs, GaN, and AlN
journal, December 1996
- Mattila, T.; Nieminen, R. M.
- Physical Review B, Vol. 54, Issue 23
Coulomb-hole summations and energies for calculations with limited number of empty orbitals: A modified static remainder approach
journal, April 2013
- Deslippe, Jack; Samsonidze, Georgy; Jain, Manish
- Physical Review B, Vol. 87, Issue 16
Native defects in Al2O3 and their impact on III-V/Al2O3 metal-oxide-semiconductor-based devices
journal, February 2011
- Weber, J. R.; Janotti, A.; Van de Walle, C. G.
- Journal of Applied Physics, Vol. 109, Issue 3
Dopant and defect energetics: Si in GaAs
journal, March 1993
- Northrup, John E.; Zhang, S. B.
- Physical Review B, Vol. 47, Issue 11
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Hybrid functionals based on a screened Coulomb potential
journal, May 2003
- Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
- The Journal of Chemical Physics, Vol. 118, Issue 18
Screened hybrid density functionals applied to solids
journal, April 2006
- Paier, J.; Marsman, M.; Hummer, K.
- The Journal of Chemical Physics, Vol. 124, Issue 15
Energy band gaps and lattice parameters evaluated with the Heyd-Scuseria-Ernzerhof screened hybrid functional
journal, November 2005
- Heyd, Jochen; Peralta, Juan E.; Scuseria, Gustavo E.
- The Journal of Chemical Physics, Vol. 123, Issue 17
Electrostatic interactions between charged defects in supercells
journal, December 2010
- Freysoldt, Christoph; Neugebauer, Jörg; Van de Walle, Chris G.
- physica status solidi (b), Vol. 248, Issue 5
BerkeleyGW: A massively parallel computer package for the calculation of the quasiparticle and optical properties of materials and nanostructures
journal, June 2012
- Deslippe, Jack; Samsonidze, Georgy; Strubbe, David A.
- Computer Physics Communications, Vol. 183, Issue 6
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009
- Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
- Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
Understanding defects in semiconductors as key to advancing device technology
journal, December 2003
- Weber, Eicke R.
- Physica B: Condensed Matter, Vol. 340-342
Theory of hydrogen diffusion and reactions in crystalline silicon
journal, May 1989
- Van de Walle, Chris G.; Denteneer, P. J. H.; Bar-Yam, Y.
- Physical Review B, Vol. 39, Issue 15
Fully Ab Initio Finite-Size Corrections for Charged-Defect Supercell Calculations
journal, January 2009
- Freysoldt, Christoph; Neugebauer, Jörg; Van de Walle, Chris G.
- Physical Review Letters, Vol. 102, Issue 1
First-principles study of fully relaxed vacancies in GaAs
journal, February 1992
- Laasonen, K.; Nieminen, R. M.; Puska, M. J.
- Physical Review B, Vol. 45, Issue 8
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
Atomic geometry and electronic structure of native defects in GaN
journal, September 1994
- Neugebauer, Jörg; Van de Walle, Chris G.
- Physical Review B, Vol. 50, Issue 11
Accuracy of for calculating defect energy levels in solids
journal, July 2017
- Chen, Wei; Pasquarello, Alfredo
- Physical Review B, Vol. 96, Issue 2
Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies
journal, October 1986
- Hybertsen, Mark S.; Louie, Steven G.
- Physical Review B, Vol. 34, Issue 8, p. 5390-5413
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
Modeling charged defects inside density functional theory band gaps
journal, May 2014
- Schultz, Peter A.; Edwards, Arthur H.
- Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 327
Density functional theory and the band gap problem
journal, March 1985
- Perdew, John P.
- International Journal of Quantum Chemistry, Vol. 28, Issue S19
Energetics of the As vacancy in GaAs: The stability of the 3+ charge state
journal, August 1994
- Northrup, John E.; Zhang, S. B.
- Physical Review B, Vol. 50, Issue 7
Theory of Carriers Transport in III-Nitride Materials: State of the Art and Future Outlook
journal, October 2013
- Bellotti, Enrico; Bertazzi, Francesco; Shishehchi, Sara
- IEEE Transactions on Electron Devices, Vol. 60, Issue 10
Computationally predicted energies and properties of defects in GaN
journal, March 2017
- Lyons, John L.; Van de Walle, Chris G.
- npj Computational Materials, Vol. 3, Issue 1
First-Principles Theory of Quasiparticles: Calculation of Band Gaps in Semiconductors and Insulators
journal, September 1985
- Hybertsen, Mark S.; Louie, Steven G.
- Physical Review Letters, Vol. 55, Issue 13
First-principles determination of defect energy levels through hybrid density functionals and GW
journal, March 2015
- Chen, Wei; Pasquarello, Alfredo
- Journal of Physics: Condensed Matter, Vol. 27, Issue 13
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
XSEDE: Accelerating Scientific Discovery
journal, September 2014
- Towns, John; Cockerill, Timothy; Dahan, Maytal
- Computing in Science & Engineering, Vol. 16, Issue 5
Charged Oxygen Defects in : Going beyond Local and Semilocal Approximations to Density Functional Theory
journal, February 2010
- Martin-Samos, L.; Roma, G.; Rinke, P.
- Physical Review Letters, Vol. 104, Issue 7
The electronic structure of impurities and other point defects in semiconductors
journal, October 1978
- Pantelides, Sokrates T.
- Reviews of Modern Physics, Vol. 50, Issue 4
Role of nitrogen vacancies in the luminescence of Mg-doped GaN
journal, April 2012
- Yan, Qimin; Janotti, Anderson; Scheffler, Matthias
- Applied Physics Letters, Vol. 100, Issue 14
Theoretical Evidence for an Optically Inducible Structural Transition of the Isolated As Antisite in GaAs: Identification and Explanation of ?
journal, May 1988
- Dabrowski, Jaroslaw; Scheffler, Matthias
- Physical Review Letters, Vol. 60, Issue 21
Green luminescence in Mg-doped GaN
journal, July 2014
- Reshchikov, M. A.; Demchenko, D. O.; McNamara, J. D.
- Physical Review B, Vol. 90, Issue 3
A hybrid density functional study of lithium in ZnO: Stability, ionization levels, and diffusion
journal, November 2009
- Carvalho, A.; Alkauskas, A.; Pasquarello, Alfredo
- Physical Review B, Vol. 80, Issue 19
Fundamental energy gap of GaN from photoluminescence excitation spectra
journal, July 1974
- Monemar, B.
- Physical Review B, Vol. 10, Issue 2
Properties of the yellow luminescence in undoped GaN epitaxial layers
journal, December 1995
- Hofmann, D. M.; Kovalev, D.; Steude, G.
- Physical Review B, Vol. 52, Issue 23
First-principles calculations of self-interstitial defect structures and diffusion paths in silicon
journal, December 1999
- Needs, R. J.
- Journal of Physics: Condensed Matter, Vol. 11, Issue 50
Oxygen and dioxygen centers in Si and Ge: Density-functional calculations
journal, October 2000
- Coutinho, J.; Jones, R.; Briddon, P. R.
- Physical Review B, Vol. 62, Issue 16
Migration mechanisms and diffusion barriers of carbon and native point defects in GaN
journal, June 2016
- Kyrtsos, Alexandros; Matsubara, Masahiko; Bellotti, Enrico
- Physical Review B, Vol. 93, Issue 24
Efficient pseudopotentials for plane-wave calculations
journal, January 1991
- Troullier, N.; Martins, José Luriaas
- Physical Review B, Vol. 43, Issue 3
Diffusivity of native defects in GaN
journal, January 2004
- Limpijumnong, Sukit; Van de Walle, Chris
- Physical Review B, Vol. 69, Issue 3
First-principles calculation of band offsets, optical bowings, and defects in CdS, CdSe, CdTe, and their alloys
journal, February 2000
- Wei, Su-Huai; Zhang, S. B.; Zunger, Alex
- Journal of Applied Physics, Vol. 87, Issue 3
The Theory of Electronic Semi-Conductors. II
journal, November 1931
- Wilson, A. H.
- Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 134, Issue 823
New Perspective on Formation Energies and Energy Levels of Point Defects in Nonmetals
journal, February 2012
- Ramprasad, R.; Zhu, H.; Rinke, Patrick
- Physical Review Letters, Vol. 108, Issue 6
Charged point defects in semiconductors
journal, December 2006
- Seebauer, Edmund G.; Kratzer, Meredith C.
- Materials Science and Engineering: R: Reports, Vol. 55, Issue 3-6
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
Neutral‐donor‐bound exciton recombination dynamics in GaN grown by metalorganic chemical vapor deposition
journal, September 1995
- Chen, G. D.; Smith, M.; Lin, J. Y.
- Applied Physics Letters, Vol. 67, Issue 12
Band-edge problem in the theoretical determination of defect energy levels: The O vacancy in ZnO as a benchmark case
journal, September 2011
- Alkauskas, Audrius; Pasquarello, Alfredo
- Physical Review B, Vol. 84, Issue 12
Native Point Defects in GaN: A Hybrid-Functional Study
journal, December 2016
- Diallo, I. C.; Demchenko, D. O.
- Physical Review Applied, Vol. 6, Issue 6
Self-compensation due to point defects in Mg-doped GaN
journal, April 2016
- Miceli, Giacomo; Pasquarello, Alfredo
- Physical Review B, Vol. 93, Issue 16
A first-principles study of carbon-related energy levels in GaN. II. Complexes formed by carbon and hydrogen, silicon or oxygen
journal, May 2017
- Matsubara, Masahiko; Bellotti, Enrico
- Journal of Applied Physics, Vol. 121, Issue 19
The energy and elastic dipole tensor of defects in ionic crystals calculated by the supercell method
journal, February 1985
- Leslie, M.; Gillan, N. J.
- Journal of Physics C: Solid State Physics, Vol. 18, Issue 5
Theory of the Atomic and Electronic Structure of Centers in GaAs and Alloys
journal, August 1988
- Chadi, D. J.; Chang, K. J.
- Physical Review Letters, Vol. 61, Issue 7
Shallow versus Deep Nature of Mg Acceptors in Nitride Semiconductors
journal, April 2012
- Lyons, John L.; Janotti, Anderson; Van de Walle, Chris G.
- Physical Review Letters, Vol. 108, Issue 15
New Method for Calculating the One-Particle Green's Function with Application to the Electron-Gas Problem
journal, August 1965
- Hedin, Lars
- Physical Review, Vol. 139, Issue 3A
Energetics and metastability of the silicon vacancy in cubic SiC
journal, April 2011
- Bruneval, Fabien; Roma, Guido
- Physical Review B, Vol. 83, Issue 14
Quasiparticle Corrections to the Electronic Properties of Anion Vacancies at GaAs(110) and InP(110)
journal, November 2006
- Hedström, Magnus; Schindlmayr, Arno; Schwarz, Günther
- Physical Review Letters, Vol. 97, Issue 22
Intrinsic defects in ZnO calculated by screened exchange and hybrid density functionals
journal, March 2010
- Clark, S. J.; Robertson, J.; Lany, S.
- Physical Review B, Vol. 81, Issue 11
A first-principles study of carbon-related energy levels in GaN. I. Complexes formed by substitutional/interstitial carbons and gallium/nitrogen vacancies
journal, May 2017
- Matsubara, Masahiko; Bellotti, Enrico
- Journal of Applied Physics, Vol. 121, Issue 19
Yellow Luminescence of Gallium Nitride Generated by Carbon Defect Complexes
journal, February 2013
- Demchenko, D. O.; Diallo, I. C.; Reshchikov, M. A.
- Physical Review Letters, Vol. 110, Issue 8
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
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
Carbon impurities and the yellow luminescence in GaN
journal, October 2010
- Lyons, J. L.; Janotti, A.; Van de Walle, C. G.
- Applied Physics Letters, Vol. 97, Issue 15
Defect-Related Donors, Acceptors, and Traps in GaN
journal, November 2001
- Look, D. C.
- physica status solidi (b), Vol. 228, Issue 1
Periodic boundary conditions in ab initio calculations. II. Brillouin-zone sampling for aperiodic systems
journal, June 1996
- Makov, G.; Shah, R.; Payne, M. C.
- Physical Review B, Vol. 53, Issue 23
Defect levels through hybrid density functionals: Insights and applications
journal, March 2011
- Alkauskas, Audrius; Broqvist, Peter; Pasquarello, Alfredo
- physica status solidi (b), Vol. 248, Issue 4
Interactions of hydrogen with native defects in GaN
journal, October 1997
- Van de Walle, Chris G.
- Physical Review B, Vol. 56, Issue 16
Luminescence properties of defects in GaN
journal, March 2005
- Reshchikov, Michael A.; Morkoç, Hadis
- Journal of Applied Physics, Vol. 97, Issue 6
Ground State of the Electron Gas by a Stochastic Method
journal, August 1980
- Ceperley, D. M.; Alder, B. J.
- Physical Review Letters, Vol. 45, Issue 7, p. 566-569
Nitrogen Vacancies as Major Point Defects in Gallium Nitride
journal, May 2006
- Ganchenkova, M. G.; Nieminen, R. M.
- Physical Review Letters, Vol. 96, Issue 19
Deep versus Shallow Behavior of Intrinsic Defects in Rutile and Anatase TiO 2 Polymorphs
journal, November 2010
- Mattioli, Giuseppe; Alippi, Paola; Filippone, Francesco
- The Journal of Physical Chemistry C, Vol. 114, Issue 49
Elastic constants of gallium nitride
journal, March 1996
- Polian, A.; Grimsditch, M.; Grzegory, I.
- Journal of Applied Physics, Vol. 79, Issue 6
Electron removal energies in Kohn-Sham density-functional theory
journal, November 1982
- Perdew, John P.; Norman, Michael R.
- Physical Review B, Vol. 26, Issue 10
Major deep levels with the same microstructures observed in n-type 4H–SiC and 6H–SiC
journal, January 2011
- Sasaki, S.; Kawahara, K.; Feng, G.
- Journal of Applied Physics, Vol. 109, Issue 1
First-principles study of oxygen vacancies in rutile
journal, February 2014
- Malashevich, Andrei; Jain, Manish; Louie, Steven G.
- Physical Review B, Vol. 89, Issue 7
Analysis of the Heyd-Scuseria-Ernzerhof density functional parameter space
journal, May 2012
- Moussa, Jonathan E.; Schultz, Peter A.; Chelikowsky, James R.
- The Journal of Chemical Physics, Vol. 136, Issue 20
Quantitative molecular orbital energies within a G0W0 approximation
journal, September 2012
- Sharifzadeh, S.; Tamblyn, I.; Doak, P.
- The European Physical Journal B, Vol. 85, Issue 9
Isolated arsenic-antisite defect in GaAs and the properties of EL 2
journal, November 1989
- Dabrowski, Jaroslaw; Scheffler, Matthias
- Physical Review B, Vol. 40, Issue 15
Quasiparticle Excitations and Charge Transition Levels of Oxygen Vacancies in Hafnia
journal, November 2011
- Jain, Manish; Chelikowsky, James R.; Louie, Steven G.
- Physical Review Letters, Vol. 107, Issue 21
Correspondence of defect energy levels in hybrid density functional theory and many-body perturbation theory
journal, September 2013
- Chen, Wei; Pasquarello, Alfredo
- Physical Review B, Vol. 88, Issue 11
A Fourfold Coordinated Point Defect in Silicon
journal, May 2002
- Goedecker, Stefan; Deutsch, Thierry; Billard, Luc
- Physical Review Letters, Vol. 88, Issue 23