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

Title: Unusual Formation of Point-Defect Complexes in the Ultrawide-Band-Gap Semiconductor β Ga 2 O 3

Abstract

Understanding the unique properties of ultra-wide band gap semiconductors requires detailed information about the exact nature of point defects and their role in determining the properties. Here, we report the first direct microscopic observation of an unusual formation of point defect complexes within the atomic-scale structure of β-Ga2O3 using high resolution scanning transmission electron microscopy (STEM). Each complex involves one cation interstitial atom paired with two cation vacancies. These divacancy-interstitial complexes correlate directly with structures obtained by density functional theory, which predicts them to be compensating acceptors in β-Ga2O3. This prediction is confirmed by a comparison between STEM data and deep level optical spectroscopy results, which reveals that these complexes correspond to a deep trap within the band gap, and that the development of the complexes is facilitated by Sn doping through increased vacancy concentration. These findings provide new insight on this emerging material’s unique response to the incorporation of impurities that can critically influence their properties.

Authors:
; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE National Nuclear Security Administration (NNSA); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); Defence Threat Reduction Agency (DTRA)
OSTI Identifier:
1573293
Alternate Identifier(s):
OSTI ID: 1863689
Report Number(s):
LLNL-JRNL-832615
Journal ID: ISSN 2160-3308; PRXHAE; 041027
Grant/Contract Number:  
AC52-07NA27344; FA9550-18-1-0479; DMR-1539918; DMR-1719875; DMR-1429155; HDTRA1-17-1-0034
Resource Type:
Published Article
Journal Name:
Physical Review. X
Additional Journal Information:
Journal Name: Physical Review. X Journal Volume: 9 Journal Issue: 4; Journal ID: ISSN 2160-3308
Publisher:
American Physical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; dopants; interstitials; point defects; vacancies

Citation Formats

Johnson, Jared M., Chen, Zhen, Varley, Joel B., Jackson, Christine M., Farzana, Esmat, Zhang, Zeng, Arehart, Aaron R., Huang, Hsien-Lien, Genc, Arda, Ringel, Steven A., Van de Walle, Chris G., Muller, David A., and Hwang, Jinwoo. Unusual Formation of Point-Defect Complexes in the Ultrawide-Band-Gap Semiconductor β − Ga 2 O 3. United States: N. p., 2019. Web. doi:10.1103/PhysRevX.9.041027.
Johnson, Jared M., Chen, Zhen, Varley, Joel B., Jackson, Christine M., Farzana, Esmat, Zhang, Zeng, Arehart, Aaron R., Huang, Hsien-Lien, Genc, Arda, Ringel, Steven A., Van de Walle, Chris G., Muller, David A., & Hwang, Jinwoo. Unusual Formation of Point-Defect Complexes in the Ultrawide-Band-Gap Semiconductor β − Ga 2 O 3. United States. https://doi.org/10.1103/PhysRevX.9.041027
Johnson, Jared M., Chen, Zhen, Varley, Joel B., Jackson, Christine M., Farzana, Esmat, Zhang, Zeng, Arehart, Aaron R., Huang, Hsien-Lien, Genc, Arda, Ringel, Steven A., Van de Walle, Chris G., Muller, David A., and Hwang, Jinwoo. Wed . "Unusual Formation of Point-Defect Complexes in the Ultrawide-Band-Gap Semiconductor β − Ga 2 O 3". United States. https://doi.org/10.1103/PhysRevX.9.041027.
@article{osti_1573293,
title = {Unusual Formation of Point-Defect Complexes in the Ultrawide-Band-Gap Semiconductor β − Ga 2 O 3},
author = {Johnson, Jared M. and Chen, Zhen and Varley, Joel B. and Jackson, Christine M. and Farzana, Esmat and Zhang, Zeng and Arehart, Aaron R. and Huang, Hsien-Lien and Genc, Arda and Ringel, Steven A. and Van de Walle, Chris G. and Muller, David A. and Hwang, Jinwoo},
abstractNote = {Understanding the unique properties of ultra-wide band gap semiconductors requires detailed information about the exact nature of point defects and their role in determining the properties. Here, we report the first direct microscopic observation of an unusual formation of point defect complexes within the atomic-scale structure of β-Ga2O3 using high resolution scanning transmission electron microscopy (STEM). Each complex involves one cation interstitial atom paired with two cation vacancies. These divacancy-interstitial complexes correlate directly with structures obtained by density functional theory, which predicts them to be compensating acceptors in β-Ga2O3. This prediction is confirmed by a comparison between STEM data and deep level optical spectroscopy results, which reveals that these complexes correspond to a deep trap within the band gap, and that the development of the complexes is facilitated by Sn doping through increased vacancy concentration. These findings provide new insight on this emerging material’s unique response to the incorporation of impurities that can critically influence their properties.},
doi = {10.1103/PhysRevX.9.041027},
journal = {Physical Review. X},
number = 4,
volume = 9,
place = {United States},
year = {2019},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1103/PhysRevX.9.041027

Citation Metrics:
Cited by: 7 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Hydrogenated cation vacancies in semiconducting oxides
journal, August 2011


Impact of proton irradiation on conductivity and deep level defects in β-Ga 2 O 3
journal, February 2019

  • Ingebrigtsen, M. E.; Kuznetsov, A. Yu.; Svensson, B. G.
  • APL Materials, Vol. 7, Issue 2
  • DOI: 10.1063/1.5054826

Atomic-scale imaging of nanoengineered oxygen vacancy profiles in SrTiO3
journal, August 2004

  • Muller, David A.; Nakagawa, Naoyuki; Ohtomo, Akira
  • Nature, Vol. 430, Issue 7000
  • DOI: 10.1038/nature02756

Electrical conductivity and carrier concentration control in β-Ga2O3 by Si doping
journal, May 2008

  • Víllora, Encarnación G.; Shimamura, Kiyoshi; Yoshikawa, Yukio
  • Applied Physics Letters, Vol. 92, Issue 20
  • DOI: 10.1063/1.2919728

Optical Absorption and Photoconductivity in the Band Edge of β Ga 2 O 3
journal, October 1965


Recent progress in Ga 2 O 3 power devices
journal, January 2016

  • Higashiwaki, Masataka; Sasaki, Kohei; Murakami, Hisashi
  • Semiconductor Science and Technology, Vol. 31, Issue 3
  • DOI: 10.1088/0268-1242/31/3/034001

Computational identification of Ga-vacancy related electron paramagnetic resonance centers in β -Ga 2 O 3
journal, May 2019

  • Skachkov, Dmitry; Lambrecht, Walter R. L.; von Bardeleben, Hans Jürgen
  • Journal of Applied Physics, Vol. 125, Issue 18
  • DOI: 10.1063/1.5092626

Editors' Choice—Hydrogen Centers in β-Ga 2 O 3 : Infrared Spectroscopy and Density Functional Theory
journal, January 2019

  • Qin, Ying; Stavola, Michael; Fowler, W. Beall
  • ECS Journal of Solid State Science and Technology, Vol. 8, Issue 7
  • DOI: 10.1149/2.0221907jss

β -(Al x Ga 1−x ) 2 O 3 /Ga 2 O 3 (010) heterostructures grown on β -Ga 2 O 3 (010) substrates by plasma-assisted molecular beam epitaxy
journal, July 2015

  • Kaun, Stephen W.; Wu, Feng; Speck, James S.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 33, Issue 4
  • DOI: 10.1116/1.4922340

Gallium oxide (Ga 2 O 3 ) metal-semiconductor field-effect transistors on single-crystal β-Ga 2 O 3 (010) substrates
journal, January 2012

  • Higashiwaki, Masataka; Sasaki, Kohei; Kuramata, Akito
  • Applied Physics Letters, Vol. 100, Issue 1
  • DOI: 10.1063/1.3674287

Depletion-mode Ga 2 O 3 metal-oxide-semiconductor field-effect transistors on β-Ga 2 O 3 (010) substrates and temperature dependence of their device characteristics
journal, September 2013

  • Higashiwaki, Masataka; Sasaki, Kohei; Kamimura, Takafumi
  • Applied Physics Letters, Vol. 103, Issue 12
  • DOI: 10.1063/1.4821858

Simulation of annular dark field stem images using a modified multislice method
journal, January 1987


Three-Dimensional Imaging of Individual Dopant Atoms in SrTiO 3
journal, December 2013


Defect phase diagram for doping of Ga 2 O 3
journal, April 2018


High-quality β-Ga 2 O 3 single crystals grown by edge-defined film-fed growth
journal, November 2016

  • Kuramata, Akito; Koshi, Kimiyoshi; Watanabe, Shinya
  • Japanese Journal of Applied Physics, Vol. 55, Issue 12
  • DOI: 10.7567/JJAP.55.1202A2

Current status of Ga 2 O 3 power devices
journal, November 2016

  • Higashiwaki, Masataka; Murakami, Hisashi; Kumagai, Yoshinao
  • Japanese Journal of Applied Physics, Vol. 55, Issue 12
  • DOI: 10.7567/JJAP.55.1202A1

Si-Ion Implantation Doping in β-Ga 2 O 3 and Its Application to Fabrication of Low-Resistance Ohmic Contacts
journal, August 2013

  • Sasaki, Kohei; Higashiwaki, Masataka; Kuramata, Akito
  • Applied Physics Express, Vol. 6, Issue 8
  • DOI: 10.7567/APEX.6.086502

Deep level defects throughout the bandgap of (010) β-Ga 2 O 3 detected by optically and thermally stimulated defect spectroscopy
journal, February 2016

  • Zhang, Z.; Farzana, E.; Arehart, A. R.
  • Applied Physics Letters, Vol. 108, Issue 5
  • DOI: 10.1063/1.4941429

Direct Observation of Sr Vacancies in SrTiO 3 by Quantitative Scanning Transmission Electron Microscopy
journal, December 2016


Oxygen vacancies and donor impurities in β-Ga2O3
journal, October 2010

  • Varley, J. B.; Weber, J. R.; Janotti, A.
  • Applied Physics Letters, Vol. 97, Issue 14
  • DOI: 10.1063/1.3499306

Migration mechanisms and diffusion barriers of vacancies in Ga 2 O 3
journal, June 2017


Position averaged convergent beam electron diffraction: Theory and applications
journal, January 2010


Czochralski growth and characterization of β-Ga2O3 single crystals
journal, August 2010

  • Galazka, Z.; Uecker, R.; Irmscher, K.
  • Crystal Research and Technology, Vol. 45, Issue 12
  • DOI: 10.1002/crat.201000341

Impact of deep level defects induced by high energy neutron radiation in β-Ga 2 O 3
journal, February 2019

  • Farzana, Esmat; Chaiken, Max F.; Blue, Thomas E.
  • APL Materials, Vol. 7, Issue 2
  • DOI: 10.1063/1.5054606

Optically and thermally detected deep levels in n -type Schottky and p+-n GaN diodes
journal, May 2000

  • Hierro, A.; Kwon, D.; Ringel, S. A.
  • Applied Physics Letters, Vol. 76, Issue 21
  • DOI: 10.1063/1.126580

Structure and vibrational properties of the dominant O-H center in β-Ga 2 O 3
journal, June 2018

  • Weiser, Philip; Stavola, Michael; Fowler, W. Beall
  • Applied Physics Letters, Vol. 112, Issue 23
  • DOI: 10.1063/1.5029921

Perspective—Opportunities and Future Directions for Ga 2 O 3
journal, January 2017

  • Mastro, Michael A.; Kuramata, Akito; Calkins, Jacob
  • ECS Journal of Solid State Science and Technology, Vol. 6, Issue 5
  • DOI: 10.1149/2.0031707jss

Atomically resolved silicon donor states of β-Ga2O3
journal, April 2011

  • Iwaya, K.; Shimizu, R.; Aida, H.
  • Applied Physics Letters, Vol. 98, Issue 14
  • DOI: 10.1063/1.3578195

Influence of incoherent twin boundaries on the electrical properties of β-Ga 2 O 3 layers homoepitaxially grown by metal-organic vapor phase epitaxy
journal, October 2017

  • Fiedler, A.; Schewski, R.; Baldini, M.
  • Journal of Applied Physics, Vol. 122, Issue 16
  • DOI: 10.1063/1.4993748

Behaviour of hydrogen in wide band gap oxides
journal, May 2014

  • Li, H.; Robertson, J.
  • Journal of Applied Physics, Vol. 115, Issue 20
  • DOI: 10.1063/1.4878415

Influence of metal choice on (010) β-Ga 2 O 3 Schottky diode properties
journal, May 2017

  • Farzana, Esmat; Zhang, Zeng; Paul, Pran K.
  • Applied Physics Letters, Vol. 110, Issue 20
  • DOI: 10.1063/1.4983610

Editors' Choice—Si- and Sn-Doped Homoepitaxial β-Ga 2 O 3 Layers Grown by MOVPE on (010)-Oriented Substrates
journal, October 2016

  • Baldini, Michele; Albrecht, Martin; Fiedler, Andreas
  • ECS Journal of Solid State Science and Technology, Vol. 6, Issue 2
  • DOI: 10.1149/2.0081702jss

Role of self-trapping in luminescence and p -type conductivity of wide-band-gap oxides
journal, February 2012


Gallium vacancies in β-Ga 2 O 3 crystals
journal, May 2017

  • Kananen, B. E.; Halliburton, L. E.; Stevens, K. T.
  • Applied Physics Letters, Vol. 110, Issue 20
  • DOI: 10.1063/1.4983814

Proton irradiation induced defects in β-Ga 2 O 3 : A combined EPR and theory study
journal, February 2019

  • von Bardeleben, Hans Jürgen; Zhou, Shengqiang; Gerstmann, Uwe
  • APL Materials, Vol. 7, Issue 2
  • DOI: 10.1063/1.5053158

Effects of crystallinity and point defects on optoelectronic applications of β-Ga_2O_3 epilayers
journal, January 2013

  • Ravadgar, Parvaneh; Horng, Ray-Hua; Yao, Shu-De
  • Optics Express, Vol. 21, Issue 21
  • DOI: 10.1364/OE.21.024599

Donors and deep acceptors in β-Ga 2 O 3
journal, August 2018

  • Neal, Adam T.; Mou, Shin; Rafique, Subrina
  • Applied Physics Letters, Vol. 113, Issue 6
  • DOI: 10.1063/1.5034474

Recent advances in free-standing single crystalline wide band-gap semiconductors and their applications: GaN, SiC, ZnO, β-Ga 2 O 3 , and diamond
journal, January 2017

  • Kim, Munho; Seo, Jung-Hun; Singisetti, Uttam
  • Journal of Materials Chemistry C, Vol. 5, Issue 33
  • DOI: 10.1039/C7TC02221B

Characterization of defects in β-Ga 2 O 3 single crystals
journal, April 2015

  • Nakai, Katsuhiko; Nagai, Tetsuya; Noami, Kengo
  • Japanese Journal of Applied Physics, Vol. 54, Issue 5
  • DOI: 10.7567/JJAP.54.051103

State-of-the-art technologies of gallium oxide power devices
journal, July 2017

  • Higashiwaki, Masataka; Kuramata, Akito; Murakami, Hisashi
  • Journal of Physics D: Applied Physics, Vol. 50, Issue 33
  • DOI: 10.1088/1361-6463/aa7aff

Electrical compensation by Ga vacancies in Ga 2 O 3 thin films
journal, June 2015

  • Korhonen, E.; Tuomisto, F.; Gogova, D.
  • Applied Physics Letters, Vol. 106, Issue 24
  • DOI: 10.1063/1.4922814

Luminescence properties of defects in GaN
journal, March 2005

  • Reshchikov, Michael A.; Morkoç, Hadis
  • Journal of Applied Physics, Vol. 97, Issue 6
  • DOI: 10.1063/1.1868059

Development of gallium oxide power devices: Development of gallium oxide power devices
journal, November 2013

  • Higashiwaki, Masataka; Sasaki, Kohei; Kuramata, Akito
  • physica status solidi (a), Vol. 211, Issue 1
  • DOI: 10.1002/pssa.201330197

Dopant activation in Sn-doped Ga 2 O 3 investigated by X-ray absorption spectroscopy
journal, December 2015

  • Siah, S. C.; Brandt, R. E.; Lim, K.
  • Applied Physics Letters, Vol. 107, Issue 25
  • DOI: 10.1063/1.4938123

Ab initio calculations on the defect structure of β -Ga 2 O 3
journal, June 2013


Synthesis and control of conductivity of ultraviolet transmitting β-Ga2O3 single crystals
journal, June 1997

  • Ueda, Naoyuki; Hosono, Hideo; Waseda, Ryuta
  • Applied Physics Letters, Vol. 70, Issue 26
  • DOI: 10.1063/1.119233

Atomic-scale imaging of individual dopant atoms and clusters in highly n-type bulk Si
journal, April 2002

  • Voyles, P. M.; Muller, D. A.; Grazul, J. L.
  • Nature, Vol. 416, Issue 6883
  • DOI: 10.1038/416826a

Deep-ultraviolet transparent conductive β-Ga2O3 thin films
journal, December 2000

  • Orita, Masahiro; Ohta, Hiromichi; Hirano, Masahiro
  • Applied Physics Letters, Vol. 77, Issue 25
  • DOI: 10.1063/1.1330559

Wide-bandgap semiconductor materials: For their full bloom
journal, February 2015