Using ground state and excited state density functional theory to decipher 3d dopant defects in GaN

Schultz, Peter A.; Lutz, Jesse J.

doi:10.1088/1361-648x/ad7fb1

Title: Using ground state and excited state density functional theory to decipher 3d dopant defects in GaN

Journal Article · 13 October 2024 · Journal of Physics. Condensed Matter

DOI: https://doi.org/10.1088/1361-648x/ad7fb1 · OSTI ID:2466295

^[1];

^[1]

Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Using ground state density functional theory (DFT) and implementing an occupation-constrained DFT (occ-DFT) for self-consistent excited state calculations, we decipher the electronic structure of the Mn dopant and other 3d defects in GaN across the band gap. Our analysis, validated with broad agreement with defect levels (ground-state calculations) and photoluminescence data (excited-state calculations), mandates reinterpretation and reassignment of 3d defect data in GaN. The Mn_Ga defect is determined to span stable charge states from (1-) in n-type GaN through (2+) in p-type GaN. The Mn(2+) is predicted to be a d² ground state spin triplet defect with a singlet excited state, isoelectronic with the defect associated with the 1.19 eV photoluminescence in n-type GaN. The combined analysis of defect levels and excited states invites reassessment of all d²-capable dopants in GaN. We demonstrate that the 1.19 eV defect, a candidate defect for optically controlled quantum applications, cannot be the Cr(1+) assumed in literature and instead must be the V(0). The combined ground-state/excited-state DFT analysis is shown to be able to chemically fingerprint defects.

View Journal Article

Cite

Export

Save

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: NA0003525

OSTI ID:: 2466295

Report Number(s):: SAND--2024-14428J

Journal Information:: Journal of Physics. Condensed Matter, Journal Name: Journal of Physics. Condensed Matter Journal Issue: 1 Vol. 37; ISSN 0953-8984

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

References (33)

Electronic structure of transition metal ions in GaN and AlN: Comparing GGA+U with experiment Zakrzewski, T.; Boguslawski, P. Journal of Alloys and Compounds, Vol. 664 https://doi.org/10.1016/j.jallcom.2015.12.258	journal	April 2016
Semi-insulating GaN substrates for high-frequency device fabrication Freitas, J. A.; Gowda, M.; Tischler, J. G. Journal of Crystal Growth, Vol. 310, Issue 17 https://doi.org/10.1016/j.jcrysgro.2008.06.038	journal	August 2008
Basic ammonothermal growth of Gallium Nitride – State of the art, challenges, perspectives Zajac, M.; Kucharski, R.; Grabianska, K. Progress in Crystal Growth and Characterization of Materials, Vol. 64, Issue 3 https://doi.org/10.1016/j.pcrysgrow.2018.05.001	journal	September 2018
Constrained Density Functional Theory Kaduk, Benjamin; Kowalczyk, Tim; Van Voorhis, Troy Chemical Reviews, Vol. 112, Issue 1 https://doi.org/10.1021/cr200148b	journal	November 2011
Manipulating Mn–Mgk cation complexes to control the charge- and spin-state of Mn in GaN Devillers, Thibaut; Rovezzi, Mauro; Szwacki, Nevill Gonzalez Scientific Reports, Vol. 2, Issue 1 https://doi.org/10.1038/srep00722	journal	October 2012
Photoluminescence of residual transition metal impurities in GaN Baur, J.; Kaufmann, U.; Kunzer, M. Applied Physics Letters, Vol. 67, Issue 8 https://doi.org/10.1063/1.114987	journal	August 1995
Optical properties of the deep Mn acceptor in GaN:Mn Korotkov, R. Y.; Gregie, J. M.; Wessels, B. W. Applied Physics Letters, Vol. 80, Issue 10 https://doi.org/10.1063/1.1456544	journal	March 2002
The Mn3+/2+ acceptor level in group III nitrides Graf, T.; Gjukic, M.; Brandt, M. S. Applied Physics Letters, Vol. 81, Issue 27 https://doi.org/10.1063/1.1530374	journal	December 2002
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
Optical properties of Mn4+ ions in GaN:Mn codoped with Mg acceptors Han, B.; Korotkov, R. Y.; Wessels, B. W. Applied Physics Letters, Vol. 84, Issue 26 https://doi.org/10.1063/1.1766082	journal	June 2004
Optical investigation of electronic states of Mn4+ ions in p-type GaN Han, B.; Wessels, B. W.; Ulmer, M. P. Applied Physics Letters, Vol. 86, Issue 4 https://doi.org/10.1063/1.1853525	journal	January 2005
Quantum computing with defects Weber, J. R.; Koehl, W. F.; Varley, J. B. Proceedings of the National Academy of Sciences, Vol. 107, Issue 19 https://doi.org/10.1073/pnas.1003052107	journal	April 2010
The E 1– E 2 center in gallium arsenide is the divacancy Schultz, Peter A. Journal of Physics: Condensed Matter, Vol. 27, Issue 7 https://doi.org/10.1088/0953-8984/27/7/075801	journal	January 2015
Simple intrinsic defects in gallium arsenide Schultz, Peter A.; von Lilienfeld, O. Anatole Modelling and Simulation in Materials Science and Engineering, Vol. 17, Issue 8 https://doi.org/10.1088/0965-0393/17/8/084007	journal	November 2009
Symmetry in density-functional theory Görling, Andreas Physical Review A, Vol. 47, Issue 4 https://doi.org/10.1103/PhysRevA.47.2783	journal	April 1993
Density-functional theory beyond the Hohenberg-Kohn theorem Görling, Andreas Physical Review A, Vol. 59, Issue 5 https://doi.org/10.1103/PhysRevA.59.3359	journal	May 1999
Theoretical study of intrinsic defects in cubic silicon carbide 3 C -SiC Schultz, Peter A.; Van Ginhoven, Renee M.; Edwards, Arthur H. Physical Review B, Vol. 103, Issue 19 https://doi.org/10.1103/PhysRevB.103.195202	journal	May 2021
Electronic structure of intrinsic defects in c -gallium nitride: Density functional theory study without the jellium approximation Edwards, Arthur H.; Schultz, Peter A.; Dobzynski, Richard M. Physical Review B, Vol. 105, Issue 23 https://doi.org/10.1103/PhysRevB.105.235110	journal	June 2022
Theory of magnetic 3d transition metal dopants in gallium nitride Schultz, Peter A.; Edwards, Arthur H.; Van Ginhoven, Renee M. Physical Review B, Vol. 107, Issue 20 https://doi.org/10.1103/PhysRevB.107.205202	journal	May 2023
Exchange and correlation in atoms, molecules, and solids by the spin-density-functional formalism Gunnarsson, O.; Lundqvist, B. I. Physical Review B, Vol. 13, Issue 10 https://doi.org/10.1103/PhysRevB.13.4274	journal	May 1976
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
Identification of the 1.19-eV luminescence in hexagonal GaN Heitz, R.; Thurian, P.; Loa, I. Physical Review B, Vol. 52, Issue 23 https://doi.org/10.1103/PhysRevB.52.16508	journal	December 1995
Local electrostatic moments and periodic boundary conditions Schultz, Peter A. Physical Review B, Vol. 60, Issue 3 https://doi.org/10.1103/PhysRevB.60.1551	journal	July 1999
Transition metal defects in group-III nitrides: An ab initio calculation of hyperfine interactions and optical transitions Gerstmann, U.; Blumenau, A. T.; Overhof, H. Physical Review B, Vol. 63, Issue 7 https://doi.org/10.1103/PhysRevB.63.075204	journal	January 2001
Structural and electronic properties of Fe 3 + and Fe 2 + centers in GaN from optical and EPR experiments Malguth, E.; Hoffmann, A.; Gehlhoff, W. Physical Review B, Vol. 74, Issue 16 https://doi.org/10.1103/PhysRevB.74.165202	journal	October 2006
Unraveling the Jahn-Teller effect in Mn-doped GaN using the Heyd-Scuseria-Ernzerhof hybrid functional Stroppa, A.; Kresse, G. Physical Review B, Vol. 79, Issue 20 https://doi.org/10.1103/PhysRevB.79.201201	journal	May 2009
Resonant optical spectroscopy and coherent control of C r 4 + spin ensembles in SiC and GaN Koehl, William F.; Diler, Berk; Whiteley, Samuel J. Physical Review B, Vol. 95, Issue 3 https://doi.org/10.1103/PhysRevB.95.035207	journal	January 2017
Electrical and optical properties of iron in GaN, AlN, and InN Wickramaratne, Darshana; Shen, Jimmy-Xuan; Dreyer, Cyrus E. Physical Review B, Vol. 99, Issue 20 https://doi.org/10.1103/PhysRevB.99.205202	journal	May 2019
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
Charged Local Defects in Extended Systems Schultz, Peter A. Physical Review Letters, Vol. 84, Issue 9 https://doi.org/10.1103/PhysRevLett.84.1942	journal	February 2000
Theory of Defect Levels and the “Band Gap Problem” in Silicon Schultz, Peter A. Physical Review Letters, Vol. 96, Issue 24 https://doi.org/10.1103/PhysRevLett.96.246401	journal	June 2006
Dilute ferromagnetic semiconductors: Physics and spintronic structures Dietl, Tomasz; Ohno, Hideo Reviews of Modern Physics, Vol. 86, Issue 1 https://doi.org/10.1103/RevModPhys.86.187	journal	March 2014
Quantum Spintronics: Engineering and Manipulating Atom-Like Spins in Semiconductors Awschalom, D. D.; Bassett, L. C.; Dzurak, A. S. Science, Vol. 339, Issue 6124 https://doi.org/10.1126/science.1231364	journal	March 2013