What is the valence of Mn in Ga1-xMnxN?
Abstract
We investigate the current debate on the Mn valence in Ga1-xMnxN, a diluted magnetic semiconductor (DMS) with a potentially high Curie temperature. From a first-principles Wannier-function analysis, we unambiguously find the Mn valence to be close to 2+ (d5), but in a mixed spin configuration with average magnetic moments of 4μB. By integrating out high-energy degrees of freedom differently, we further derive for the first time from first-principles two low-energy pictures that reflect the intrinsic dual nature of the doped holes in the DMS: (1) an effective d4 picture ideal for local physics, and (2) an effective d5 picture suitable for extended properties. In the latter, our results further reveal a few novel physical effects, and pave the way for future realistic studies of magnetism. Our study not only resolves one of the outstanding key controversies of the field, but also exemplifies the general need for multiple effective descriptions to account for the rich low-energy physics in many-body systems in general.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Louisiana State Univ., Baton Rouge, LA (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States); State Univ. of New York, Stony Brook, NY (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1225424
- Alternate Identifier(s):
- OSTI ID: 1225231; OSTI ID: 1240596
- Report Number(s):
- BNL-111797-2016-JA
Journal ID: ISSN 0031-9007; PRLTAO
- Grant/Contract Number:
- AC05-00OR22725; AC02-98CH10886; SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Letters
- Additional Journal Information:
- Journal Volume: 115; Journal Issue: 19; Journal ID: ISSN 0031-9007
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Berlijn, Tom, Jarrell, Mark, Nelson, Ryky, Ku, Wei, and Moreno, Juana. What is the valence of Mn in Ga1-xMnxN?. United States: N. p., 2015.
Web. doi:10.1103/PhysRevLett.115.197203.
Berlijn, Tom, Jarrell, Mark, Nelson, Ryky, Ku, Wei, & Moreno, Juana. What is the valence of Mn in Ga1-xMnxN?. United States. https://doi.org/10.1103/PhysRevLett.115.197203
Berlijn, Tom, Jarrell, Mark, Nelson, Ryky, Ku, Wei, and Moreno, Juana. Wed .
"What is the valence of Mn in Ga1-xMnxN?". United States. https://doi.org/10.1103/PhysRevLett.115.197203. https://www.osti.gov/servlets/purl/1225424.
@article{osti_1225424,
title = {What is the valence of Mn in Ga1-xMnxN?},
author = {Berlijn, Tom and Jarrell, Mark and Nelson, Ryky and Ku, Wei and Moreno, Juana},
abstractNote = {We investigate the current debate on the Mn valence in Ga1-xMnxN, a diluted magnetic semiconductor (DMS) with a potentially high Curie temperature. From a first-principles Wannier-function analysis, we unambiguously find the Mn valence to be close to 2+ (d5), but in a mixed spin configuration with average magnetic moments of 4μB. By integrating out high-energy degrees of freedom differently, we further derive for the first time from first-principles two low-energy pictures that reflect the intrinsic dual nature of the doped holes in the DMS: (1) an effective d4 picture ideal for local physics, and (2) an effective d5 picture suitable for extended properties. In the latter, our results further reveal a few novel physical effects, and pave the way for future realistic studies of magnetism. Our study not only resolves one of the outstanding key controversies of the field, but also exemplifies the general need for multiple effective descriptions to account for the rich low-energy physics in many-body systems in general.},
doi = {10.1103/PhysRevLett.115.197203},
journal = {Physical Review Letters},
number = 19,
volume = 115,
place = {United States},
year = {Wed Nov 04 00:00:00 EST 2015},
month = {Wed Nov 04 00:00:00 EST 2015}
}
Web of Science
Works referenced in this record:
Mn L3,2 x-ray absorption from (Ga,Mn)As and (Ga,Mn)N
journal, June 2004
- Edmonds, K. W.; Farley, N. R. S.; Johal, T. K.
- Journal of Applied Physics, Vol. 95, Issue 11
Growth and characterization of GaN:Mn epitaxial films
journal, June 2003
- Graf, T.; Gjukic, M.; Hermann, M.
- Journal of Applied Physics, Vol. 93, Issue 12
Density-functional theory and NiO photoemission spectra
journal, December 1993
- Anisimov, V. I.; Solovyev, I. V.; Korotin, M. A.
- Physical Review B, Vol. 48, Issue 23
Optical properties of the deep Mn acceptor in GaN:Mn
journal, March 2002
- Korotkov, R. Y.; Gregie, J. M.; Wessels, B. W.
- Applied Physics Letters, Vol. 80, Issue 10
Indication of ferromagnetism in molecular-beam-epitaxy-derived N-type GaMnN
journal, August 2001
- Overberg, Mark E.; Abernathy, Cammy R.; Pearton, Stephen J.
- Applied Physics Letters, Vol. 79, Issue 9
X-ray absorption near-edge structure and valence state of Mn in (Ga,Mn)N
journal, September 2005
- Titov, A.; Biquard, X.; Halley, D.
- Physical Review B, Vol. 72, Issue 11
Effect of the location of Mn sites in ferromagnetic on its Curie temperature
journal, April 2002
- Yu, K. M.; Walukiewicz, W.; Wojtowicz, T.
- Physical Review B, Vol. 65, Issue 20
Optical properties of Mn-doped GaN
journal, January 2012
- Boukortt, A.; Hayn, R.; Virot, F.
- Physical Review B, Vol. 85, Issue 3
First-Principles Method of Propagation of Tightly Bound Excitons: Verifying the Exciton Band Structure of LiF with Inelastic x-Ray Scattering
journal, October 2013
- Lee, Chi-Cheng; Chen, Xiaoqian M.; Gan, Yu
- Physical Review Letters, Vol. 111, Issue 15
Metalorganic vapor phase epitaxial growth of a high quality GaN film using an AlN buffer layer
journal, February 1986
- Amano, H.; Sawaki, N.; Akasaki, I.
- Applied Physics Letters, Vol. 48, Issue 5, p. 353-355
Effect of low-temperature annealing on transport and magnetism of diluted magnetic semiconductor (Ga, Mn)As
journal, March 2001
- Hayashi, Takashi; Hashimoto, Yoshiaki; Katsumoto, Shingo
- Applied Physics Letters, Vol. 78, Issue 12
Magnetic properties of n -GaMnN thin films
journal, May 2002
- Thaler, G. T.; Overberg, M. E.; Gila, B.
- Applied Physics Letters, Vol. 80, Issue 21
Effect of covalent bonding on magnetism and the missing neutron intensity in copper oxide compounds
journal, October 2009
- Walters, Andrew C.; Perring, Toby G.; Caux, Jean-Sébastien
- Nature Physics, Vol. 5, Issue 12
Optical properties of III-Mn-V ferromagnetic semiconductors
journal, December 2008
- Burch, K. S.; Awschalom, D. D.; Basov, D. N.
- Journal of Magnetism and Magnetic Materials, Vol. 320, Issue 23
Demonstration of the spin solar cell and spin photodiode effect
journal, July 2013
- Endres, B.; Ciorga, M.; Schmid, M.
- Nature Communications, Vol. 4, Issue 1
Magnetic and transport characteristics on high Curie temperature ferromagnet of Mn-doped GaN
journal, January 2002
- Sasaki, Takahiko; Sonoda, Saki; Yamamoto, Yoshiyuki
- Journal of Applied Physics, Vol. 91, Issue 10
High-Curie-temperature Ga1−xMnxAs obtained by resistance-monitored annealing
journal, December 2002
- Edmonds, K. W.; Wang, K. Y.; Campion, R. P.
- Applied Physics Letters, Vol. 81, Issue 26
Electrical spin injection in a ferromagnetic semiconductor heterostructure
journal, December 1999
- Ohno, Y.; Young, D. K.; Beschoten, B.
- Nature, Vol. 402, Issue 6763
Local structure and chemical valency of Mn impurities in wide-band-gap III–V magnetic alloy semiconductors Ga1−xMnxN
journal, December 2001
- Soo, Y. L.; Kioseoglou, G.; Kim, S.
- Applied Physics Letters, Vol. 79, Issue 24
Spintronics: A Spin-Based Electronics Vision for the Future
journal, November 2001
- Wolf, S. A.; Awschalom, D. D.; Buhrman, R. A.
- Science, Vol. 294, Issue 5546, p. 1488-1495
First-Principles Study of Ferromagnetism in Mn-Doped GaN
journal, February 2005
- Kang, J.; Chang, K. J.; Katayama-Yoshida, H.
- Journal of Superconductivity, Vol. 18, Issue 1
Proposal for a spin-polarized solar battery
journal, September 2001
- Žutić, Igor; Fabian, Jaroslav; Das Sarma, S.
- Applied Physics Letters, Vol. 79, Issue 10
Nano-clusters structure and magnetic properties of high fluence Mn+ ion-implanted GaN
journal, June 2008
- Chen, Di; Ding, Zhibo; Yao, Shude
- Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 266, Issue 12-13
Candela‐class high‐brightness InGaN/AlGaN double‐heterostructure blue‐light‐emitting diodes
journal, March 1994
- Nakamura, Shuji; Mukai, Takashi; Senoh, Masayuki
- Applied Physics Letters, Vol. 64, Issue 13, p. 1687-1689
The Mn3+/2+ acceptor level in group III nitrides
journal, December 2002
- Graf, T.; Gjukic, M.; Brandt, M. S.
- Applied Physics Letters, Vol. 81, Issue 27
Exchange interactions in diluted magnetic semiconductors
journal, November 2004
- Sato, K.; Dederichs, P. H.; Katayama-Yoshida, H.
- Journal of Physics: Condensed Matter, Vol. 16, Issue 48
Local Structure and Valence State of Mn in Ga1−x Mn x N Epilayers
journal, February 2003
- Biquard, X.
- Journal of Superconductivity, Vol. 16, Issue 1, p. 127-129
Paramagnetism and antiferromagnetic d–d coupling in GaMnN magnetic semiconductor
journal, October 2001
- Zając, M.; Gosk, J.; Kamińska, M.
- Applied Physics Letters, Vol. 79, Issue 15
Theory of magnetic anisotropy in ferromagnets
journal, January 2001
- Abolfath, M.; Jungwirth, T.; Brum, J.
- Physical Review B, Vol. 63, Issue 5
Room temperature ferromagnetic properties of (Ga, Mn)N
journal, November 2001
- Reed, M. L.; El-Masry, N. A.; Stadelmaier, H. H.
- Applied Physics Letters, Vol. 79, Issue 21
Ferromagnetism of ZnO and GaN: A Review
journal, September 2005
- Liu, C.; Yun, F.; Morkoç, H.
- Journal of Materials Science: Materials in Electronics, Vol. 16, Issue 9
Electronic structure, magnetic ordering, and optical properties of GaN and GaAs doped with Mn
journal, July 2002
- Kulatov, E.; Nakayama, H.; Mariette, H.
- Physical Review B, Vol. 66, Issue 4
Dynamical reconstruction of the exciton in LiF with inelastic x-ray scattering
journal, August 2008
- Abbamonte, P.; Graber, T.; Reed, J. P.
- Proceedings of the National Academy of Sciences, Vol. 105, Issue 34
Spintronics: Fundamentals and applications
journal, April 2004
- Žutić, Igor; Fabian, Jaroslav; Das Sarma, S.
- Reviews of Modern Physics, Vol. 76, Issue 2
Wide bandgap GaN-based semiconductors for spintronics
journal, February 2004
- Pearton, S. J.; Abernathy, C. R.; Thaler, G. T.
- Journal of Physics: Condensed Matter, Vol. 16, Issue 7
Growth of GaN and AlGaN for UV/blue p-n junction diodes
journal, March 1993
- Akasaki, I.; Amano, H.; Murakami, H.
- Journal of Crystal Growth, Vol. 128, Issue 1-4
Hole-mediated ferromagnetism in tetrahedrally coordinated semiconductors
journal, April 2001
- Dietl, T.; Ohno, H.; Matsukura, F.
- Physical Review B, Vol. 63, Issue 19
Nearest-neighbor Mn antiferromagnetic exchange in
journal, May 2010
- Granville, S.; Ruck, B. J.; Budde, F.
- Physical Review B, Vol. 81, Issue 18
Observation of spin-glass behavior in homogeneous (Ga,Mn)N layers grown by reactive molecular-beam epitaxy
journal, April 2003
- Dhar, S.; Brandt, O.; Trampert, A.
- Physical Review B, Vol. 67, Issue 16
Phase diagram and critical behavior of the random ferromagnet Ga Mn N
journal, August 2013
- Stefanowicz, S.; Kunert, G.; Simserides, C.
- Physical Review B, Vol. 88, Issue 8
Theory of ferromagnetic (III,Mn)V semiconductors
journal, August 2006
- Jungwirth, T.; Sinova, Jairo; Mašek, J.
- Reviews of Modern Physics, Vol. 78, Issue 3
First-principles theory of dilute magnetic semiconductors
journal, May 2010
- Sato, K.; Bergqvist, L.; Kudrnovský, J.
- Reviews of Modern Physics, Vol. 82, Issue 2
Interaction Between the Shells in the Transition Metals
journal, February 1951
- Zener, C.
- Physical Review, Vol. 81, Issue 3
Weak localization in : Evidence of impurity band transport
journal, October 2007
- Rokhinson, L. P.; Lyanda-Geller, Y.; Ge, Z.
- Physical Review B, Vol. 76, Issue 16
Interaction between the -Shells in the Transition Metals. II. Ferromagnetic Compounds of Manganese with Perovskite Structure
journal, May 1951
- Zener, Clarence
- Physical Review, Vol. 82, Issue 3
Mn-related absorption and PL bands in GaN grown by metal organic vapor phase epitaxy
journal, December 2001
- Korotkov, R. Y.; Gregie, J. M.; Wessels, B. W.
- Physica B: Condensed Matter, Vol. 308-310
Electronic structure and magnetism of Mn-doped GaN
journal, November 2003
- Sanyal, B.; Bengone, O.; Mirbt, S.
- Physical Review B, Vol. 68, Issue 20
On-site Coulomb interaction and the magnetism of (GaMn)N and (GaMn)As
journal, May 2004
- Sandratskii, L. M.; Bruno, P.; Kudrnovský, J.
- Physical Review B, Vol. 69, Issue 19
Different origins of the ferromagnetic order in (Ga,Mn)As and (Ga,Mn)
journal, December 2004
- Wierzbowska, Małgorzata; Sánchez-Portal, Daniel; Sanvito, Stefano
- Physical Review B, Vol. 70, Issue 23
First-principles investigation of the assumptions underlying model-Hamiltonian approaches to ferromagnetism of impurities in III-V semiconductors
journal, March 2004
- Mahadevan, Priya; Zunger, Alex
- Physical Review B, Vol. 69, Issue 11
Electronic structure of the neutral manganese acceptor in gallium arsenide
journal, July 1987
- Schneider, J.; Kaufmann, U.; Wilkening, W.
- Physical Review Letters, Vol. 59, Issue 2
Structural and paramagnetic properties of dilute
journal, June 2010
- Stefanowicz, Wiktor; Sztenkiel, Dariusz; Faina, Bogdan
- Physical Review B, Vol. 81, Issue 23
High-energy spectroscopic study of the III-V nitride-based diluted magnetic semiconductor
journal, August 2005
- Hwang, J. I.; Ishida, Y.; Kobayashi, M.
- Physical Review B, Vol. 72, Issue 8
Insulating Ferromagnetism in : An Ab Initio Wannier Function Analysis
journal, September 2002
- Ku, Wei; Rosner, H.; Pickett, W. E.
- Physical Review Letters, Vol. 89, Issue 16
Jahn-Teller distortion and ferromagnetism in the dilute magnetic semiconductors GaAs:Mn and cubic GaN:Mn
journal, July 2005
- Luo, Xuan; Martin, Richard M.
- Physical Review B, Vol. 72, Issue 3
Nonresonant Inelastic X-Ray Scattering and Energy-Resolved Wannier Function Investigation of Excitations in NiO and CoO
journal, July 2007
- Larson, B. C.; Ku, Wei; Tischler, J. Z.
- Physical Review Letters, Vol. 99, Issue 2
Effective Hamiltonian for the superconducting Cu oxides
journal, March 1988
- Zhang, F. C.; Rice, T. M.
- Physical Review B, Vol. 37, Issue 7
Tuning the in-plane electron behavior in high- cuprate superconductors via apical atoms: A first-principles Wannier-states analysis
journal, June 2009
- Yin, Wei-Guo; Ku, Wei
- Physical Review B, Vol. 79, Issue 21
Dynamical linear response of TDDFT with functional: Strongly hybridized Frenkel excitons in NiO
journal, August 2010
- Lee, Chi-Cheng; Hsueh, H. C.; Ku, Wei
- Physical Review B, Vol. 82, Issue 8
Neutral and charged embedded clusters of Mn in doped GaN from first principles
journal, July 2007
- Cui, X. Y.; Delley, B.; Freeman, A. J.
- Physical Review B, Vol. 76, Issue 4
Absence of Diffusion in Certain Random Lattices
journal, March 1958
- Anderson, P. W.
- Physical Review, Vol. 109, Issue 5
Mechanism for high-temperature superconductivity
journal, September 1988
- Emery, V. J.; Reiter, G.
- Physical Review B, Vol. 38, Issue 7
Ferromagnetism of ZnO and GaN: A Review
journal, May 2006
- Liu, C.; Yun, F.; Morko, H.
- ChemInform, Vol. 37, Issue 21
Proposal for a spin-polarized solar battery
text, January 2001
- Zutic, Igor; Fabian, Jaroslav; Sarma, S. Das
- Universität Regensburg
Demonstration of the spin solar cell and spin photodiode effect
text, January 2013
- Endres, Bernhard; Ciorga, Mariusz; Schmid, Maximilian
- Universität Regensburg
Spintronics: fundamentals and applications
text, January 2004
- Zutic, Igor; Fabian, Jaroslav; Sarma, S. Das
- Universität Regensburg
Optical Properties of III-Mn-V Ferromagnetic Semiconductors
text, January 2008
- Burch, K. S.; Awschalom, D. D.; Basov, D. N.
- arXiv
Structural and paramagnetic properties of dilute Ga1-xMnxN
text, January 2009
- Stefanowicz, Wiktor; Sztenkiel, Dariusz; Faina, Bogdan
- arXiv
Theory of Magnetic Anisotropy in III_{1-x}Mn_{x}V Ferromagnets
text, January 2000
- Abolfath, M.; Jungwirth, T.; Brum, J.
- arXiv
Hole-mediated ferromagnetism in tetrahedrally coordinated semiconductors
text, January 2000
- Dietl, T.; Ohno, H.; Matsukura, F.
- arXiv
A proposal for a spin-polarized solar battery
text, January 2001
- Zutic, Igor; Fabian, Jaroslav; Sarma, S. Das
- arXiv
Electronic structure and magnetism of Mn doped GaN
text, January 2003
- Sanyal, B.; Bengone, O.; Mirbt, S.
- arXiv
On-site Coulomb interaction and the magnetism of (GaMn)N and (GaMn)As
text, January 2004
- Sandratskii, L. M.; Bruno, P.; Kudrnovský, J.
- arXiv
Different origin of the ferromagnetic order in (Ga,Mn)As and (Ga,Mn)N
text, January 2004
- Wierzbowska, Malgorzata; Sanchez-Portal, Daniel; Sanvito, Stefano
- arXiv
Theory of ferromagnetic (III,Mn)V semiconductors
text, January 2006
- Jungwirth, T.; Sinova, Jairo; Masek, J.
- arXiv
Works referencing / citing this record:
Diluted Magnetic Semiconductors: Basic Physics and Optical Properties
book, October 2017
- Cibert, Joël; Scalbert, Denis
- Spin Physics in Semiconductors
Systematic Quantum Cluster Typical Medium Method for the Study of Localization in Strongly Disordered Electronic Systems
journal, November 2018
- Terletska, Hanna; Zhang, Yi; Tam, Ka-Ming
- Applied Sciences, Vol. 8, Issue 12
Diluted Magnetic Semiconductors: Basic Physics and Optical Properties
book, January 2008
- Cibert, J.; Scalbert, D.
- Springer Series in Solid-State Sciences
Generalized Multiband Typical Medium Dynamical Cluster Approximation: Application to (Ga,Mn)N
text, January 2016
- Zhang, Yi; Nelson, R.; Siddiqui, Elisha
- arXiv
Systematic Quantum Cluster Typical Medium Method For the Study of Localization in Strongly Disordered Electronic Systems
text, January 2018
- Terletska, Hanna; Zhang, Yi; Tam, Ka Ming
- arXiv