DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: 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:
 [1];  [2];  [2];  [3];  [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Louisiana State Univ., Baton Rouge, LA (United States)
  3. 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}
}

Journal Article:

Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science

Save / Share:

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
  • DOI: 10.1063/1.1667419

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
  • DOI: 10.1063/1.1577811

Density-functional theory and NiO photoemission spectra
journal, December 1993


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
  • DOI: 10.1063/1.1456544

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
  • DOI: 10.1063/1.1397763

X-ray absorption near-edge structure and valence state of Mn in (Ga,Mn)N
journal, September 2005


Effect of the location of Mn sites in ferromagnetic Ga 1 x Mn x As on its Curie temperature
journal, April 2002


Optical properties of Mn-doped GaN
journal, January 2012


First-Principles Method of Propagation of Tightly Bound Excitons: Verifying the Exciton Band Structure of LiF with Inelastic x-Ray Scattering
journal, October 2013


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
  • DOI: 10.1063/1.96549

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
  • DOI: 10.1063/1.1352701

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
  • DOI: 10.1063/1.1481533

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
  • DOI: 10.1038/nphys1405

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
  • DOI: 10.1016/j.jmmm.2008.08.060

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
  • DOI: 10.1038/ncomms3068

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
  • DOI: 10.1063/1.1451879

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
  • DOI: 10.1063/1.1529079

Electrical spin injection in a ferromagnetic semiconductor heterostructure
journal, December 1999

  • Ohno, Y.; Young, D. K.; Beschoten, B.
  • Nature, Vol. 402, Issue 6763
  • DOI: 10.1038/45509

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
  • DOI: 10.1063/1.1423406

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
  • DOI: 10.1126/science.1065389

First-Principles Study of Ferromagnetism in Mn-Doped GaN
journal, February 2005


Proposal for a spin-polarized solar battery
journal, September 2001

  • Žutić, Igor; Fabian, Jaroslav; Das Sarma, S.
  • Applied Physics Letters, Vol. 79, Issue 10
  • DOI: 10.1063/1.1399002

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
  • DOI: 10.1016/j.nimb.2008.03.120

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
  • DOI: 10.1063/1.111832

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
  • DOI: 10.1063/1.1530374

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
  • DOI: 10.1088/0953-8984/16/48/003

Magnetoelectronics
journal, November 1998


Local Structure and Valence State of Mn in Ga1−x Mn x N Epilayers
journal, February 2003


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
  • DOI: 10.1063/1.1406558

Theory of magnetic anisotropy in III 1 x Mn x V ferromagnets
journal, January 2001


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
  • DOI: 10.1063/1.1419231

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
  • DOI: 10.1007/s10854-005-3232-1

Electronic structure, magnetic ordering, and optical properties of GaN and GaAs doped with Mn
journal, July 2002


Spintronics
journal, January 2001


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
  • DOI: 10.1073/pnas.0801623105

Spintronics: Fundamentals and applications
journal, April 2004


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
  • DOI: 10.1088/0953-8984/16/7/R03

Growth of GaN and AlGaN for UV/blue p-n junction diodes
journal, March 1993


Hole-mediated ferromagnetism in tetrahedrally coordinated semiconductors
journal, April 2001


Nearest-neighbor Mn antiferromagnetic exchange in Ga 1 x Mn x N
journal, May 2010


Observation of spin-glass behavior in homogeneous (Ga,Mn)N layers grown by reactive molecular-beam epitaxy
journal, April 2003


Phase diagram and critical behavior of the random ferromagnet Ga 1 x Mn x N
journal, August 2013


Theory of ferromagnetic (III,Mn)V semiconductors
journal, August 2006


First-principles theory of dilute magnetic semiconductors
journal, May 2010


Interaction Between the d Shells in the Transition Metals
journal, February 1951


Weak localization in Ga 1 x Mn x As : Evidence of impurity band transport
journal, October 2007


Mn-related absorption and PL bands in GaN grown by metal organic vapor phase epitaxy
journal, December 2001


Electronic structure and magnetism of Mn-doped GaN
journal, November 2003


On-site Coulomb interaction and the magnetism of (GaMn)N and (GaMn)As
journal, May 2004


Different origins of the ferromagnetic order in (Ga,Mn)As and (Ga,Mn) N
journal, December 2004

  • Wierzbowska, Małgorzata; Sánchez-Portal, Daniel; Sanvito, Stefano
  • Physical Review B, Vol. 70, Issue 23
  • DOI: 10.1103/PhysRevB.70.235209

Electronic structure of the neutral manganese acceptor in gallium arsenide
journal, July 1987


Structural and paramagnetic properties of dilute Ga 1 x Mn x N
journal, June 2010


High-energy spectroscopic study of the III-V nitride-based diluted magnetic semiconductor Ga 1 x Mn x N
journal, August 2005


Insulating Ferromagnetism in L a 4 B a 2 C u 2 O 10 : An Ab Initio Wannier Function Analysis
journal, September 2002


Jahn-Teller distortion and ferromagnetism in the dilute magnetic semiconductors GaAs:Mn and cubic GaN:Mn
journal, July 2005


Nonresonant Inelastic X-Ray Scattering and Energy-Resolved Wannier Function Investigation of d d Excitations in NiO and CoO
journal, July 2007


Effective Hamiltonian for the superconducting Cu oxides
journal, March 1988


Dynamical linear response of TDDFT with LDA + U functional: Strongly hybridized Frenkel excitons in NiO
journal, August 2010


Neutral and charged embedded clusters of Mn in doped GaN from first principles
journal, July 2007


Absence of Diffusion in Certain Random Lattices
journal, March 1958


Mechanism for high-temperature superconductivity
journal, September 1988


Ferromagnetism of ZnO and GaN: A Review
journal, May 2006


Proposal for a spin-polarized solar battery
text, January 2001

  • Zutic, Igor; Fabian, Jaroslav; Sarma, S. Das
  • Universität Regensburg
  • DOI: 10.5283/epub.1830

Demonstration of the spin solar cell and spin photodiode effect
text, January 2013

  • Endres, Bernhard; Ciorga, Mariusz; Schmid, Maximilian
  • Universität Regensburg
  • DOI: 10.5283/epub.28498

Spintronics: fundamentals and applications
text, January 2004

  • Zutic, Igor; Fabian, Jaroslav; Sarma, S. Das
  • Universität Regensburg
  • DOI: 10.5283/epub.1823

Optical Properties of III-Mn-V Ferromagnetic Semiconductors
text, January 2008


Structural and paramagnetic properties of dilute Ga1-xMnxN
text, January 2009


Theory of Magnetic Anisotropy in III_{1-x}Mn_{x}V Ferromagnets
text, January 2000


Hole-mediated ferromagnetism in tetrahedrally coordinated semiconductors
text, January 2000


A proposal for a spin-polarized solar battery
text, January 2001


Electronic structure and magnetism of Mn doped GaN
text, January 2003


On-site Coulomb interaction and the magnetism of (GaMn)N and (GaMn)As
text, January 2004


Different origin of the ferromagnetic order in (Ga,Mn)As and (Ga,Mn)N
text, January 2004


Theory of ferromagnetic (III,Mn)V semiconductors
text, January 2006


Works referencing / citing this record:

Diluted Magnetic Semiconductors: Basic Physics and Optical Properties
book, October 2017


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
  • DOI: 10.3390/app8122401

Diluted Magnetic Semiconductors: Basic Physics and Optical Properties
book, January 2008