Primary intrinsic defects and their charge transition levels in β–Ga2O3

Zimmermann, C.; Rønning, V.; Kalmann Frodason, Y.; Bobal, V.; Vines, L.; Varley, J. B.

doi:10.1103/physrevmaterials.4.074605

Title: Primary intrinsic defects and their charge transition levels in β–Ga₂O₃

Abstract

A steady-state photocapacitance (SSPC) setup directly connected to the beamline of a MeV ion implanter is utilized to study primary intrinsic defects in $β – {Ga}_{2} O_{3}$ generated by He implantation at cryogenic temperatures (120 K). At low temperatures, the migration of defects is suppressed, and hence the generation of primary intrinsic defects is expected to prevail. SSPC measurements reveal defect-related optical transitions in halide vapor-phase epitaxy (HVPE) -grown $β – {Ga}_{2} O_{3}$ thin films with onset energies at 1.3 $(T_{1}),$ 1.7 $(T_{2}),$ 1.9 $(T_{3}),$ 2.6 $(T_{4}),$ 3.7 $(T_{5}),$ and 4.2 eV $(T_{6})$ . $T_{2},$ $T_{4},$ $T_{5},$ and $T_{6}$ were observed in as-received HVPE-grown $β – {Ga}_{2} O_{3}$ thin films, whereby $T_{2}$ is only sporadically observed. The introduction rates for $T_{3},$ $T_{4},$ as well as $T_{6}$ indicate an origin related to primary intrinsic defects. Notably, $T_{1}$ and $T_{3}$ are only observed after He implantation at cryogenic temperatures. Hybrid-functional calculations were performed to estimate the optical absorption cross-section spectra for the gallium $({Ga}_{i})$ and oxygen $(O_{i})$ interstitials as well as the corresponding vacancies ( $V_{Ga}$ and $V_{O}$ , respectively), and compared with the measured onsets for optical absorption found by SSPC measurements. Indeed, we propose $T_{3}$ to be associated with ${Ga}_{i}^{(+ / + 2)}$ and/or $V_{GaI}^{(- 3 / - 2)}$ , while $T_{4}$ is suggested to be related to $V_{O K}^{(0 / +)}$ $(K = I, II, III)$ and/or $V_{GaII}^{(- 3 / - 2)}$ . Additionally, several further charge-state transition levels associated with $V_{GaI}$ and $V_{GaII}$ may contribute to $T_{4}$ and $T_{6}$ . We further studied the kinetics of the defects created with He implantation by exposing the sample to room temperature. The kinetics observed for $T_{3}$ and $T_{4}$ further support the proposed assignments of the corresponding defect signatures.

Authors:

^[1];

^[1]; Bobal, V. ^[1]; Vines, L. ^[1];

^[2]

Univ. of Oslo (Norway)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Publication Date:: Fri Jul 24 00:00:00 EDT 2020

Research Org.:: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1668483

Report Number(s):: LLNL-JRNL-812190
Journal ID: ISSN 2475-9953; 1000612; TRN: US2203796

Grant/Contract Number:: AC52-07NA27344

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Materials

Additional Journal Information:: Journal Volume: 4; Journal Issue: 7; Journal ID: ISSN 2475-9953

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Defects; first-principles calculations; interstitials; irradiation effects; point defects; vacancies; semiconductors; single crystal materials; wide band gap systems

Citation Formats


                    Zimmermann, C., Rønning, V., Kalmann Frodason, Y., Bobal, V., Vines, L., and Varley, J. B. Primary intrinsic defects and their charge transition levels in β–Ga2O3.  United States: N. p., 2020. 
Web.  doi:10.1103/physrevmaterials.4.074605.

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                    Zimmermann, C., Rønning, V., Kalmann Frodason, Y., Bobal, V., Vines, L., & Varley, J. B. Primary intrinsic defects and their charge transition levels in β–Ga2O3.  United States.  https://doi.org/10.1103/physrevmaterials.4.074605

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                    Zimmermann, C., Rønning, V., Kalmann Frodason, Y., Bobal, V., Vines, L., and Varley, J. B. Fri .  
"Primary intrinsic defects and their charge transition levels in β–Ga2O3".  United States.  https://doi.org/10.1103/physrevmaterials.4.074605.  https://www.osti.gov/servlets/purl/1668483.

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@article{osti_1668483,

  title        = {Primary intrinsic defects and their charge transition levels in β–Ga2O3},

  author       = {Zimmermann, C. and Rønning, V. and Kalmann Frodason, Y. and Bobal, V. and Vines, L. and Varley, J. B.},

  abstractNote = {A steady-state photocapacitance (SSPC) setup directly connected to the beamline of a MeV ion implanter is utilized to study primary intrinsic defects in β–Ga2O3 generated by He implantation at cryogenic temperatures (120 K). At low temperatures, the migration of defects is suppressed, and hence the generation of primary intrinsic defects is expected to prevail. SSPC measurements reveal defect-related optical transitions in halide vapor-phase epitaxy (HVPE) -grown β–Ga2O3 thin films with onset energies at 1.3 (T1), 1.7 (T2), 1.9 (T3), 2.6 (T4), 3.7 (T5), and 4.2 eV (T6). T2, T4, T5, and T6 were observed in as-received HVPE-grown β–Ga2O3 thin films, whereby T2 is only sporadically observed. The introduction rates for T3, T4, as well as T6 indicate an origin related to primary intrinsic defects. Notably, T1 and T3 are only observed after He implantation at cryogenic temperatures. Hybrid-functional calculations were performed to estimate the optical absorption cross-section spectra for the gallium (Gai) and oxygen (Oi) interstitials as well as the corresponding vacancies (VGa and VO, respectively), and compared with the measured onsets for optical absorption found by SSPC measurements. Indeed, we propose T3 to be associated with Gai(+/+2) and/or VGaI(-3/-2), while T4 is suggested to be related to VOK(0/+) (K=I, II, III) and/or VGaII(-3/-2). Additionally, several further charge-state transition levels associated with VGaI and VGaII may contribute to T4 and T6. We further studied the kinetics of the defects created with He implantation by exposing the sample to room temperature. The kinetics observed for T3 and T4 further support the proposed assignments of the corresponding defect signatures.},

  doi          = {10.1103/physrevmaterials.4.074605},

  journal      = {Physical Review Materials},

  number       = 7,

  volume       = 4,

  place        = {United States},

  year         = {Fri Jul 24 00:00:00 EDT 2020},

  month        = {Fri Jul 24 00:00:00 EDT 2020}

}

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Title: Primary intrinsic defects and their charge transition levels in β–Ga2O3

Abstract

Citation Formats

Hydrogenated cation vacancies in semiconducting oxides journal, August 2011

Iron and intrinsic deep level states in Ga 2 O 3 journal, January 2018

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

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Deep level defects in Ge-doped (010) β-Ga 2 O 3 layers grown by plasma-assisted molecular beam epitaxy journal, April 2018

Direct Evaluation of Defect Distributions From Admittance Spectroscopy journal, November 2014

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

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Optical evidence of intrinsic quantum wells in the transparent conducting oxide β-Ga2O3 journal, August 2000

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Fully Ab Initio Finite-Size Corrections for Charged-Defect Supercell Calculations journal, January 2009

From ultrasoft pseudopotentials to the projector augmented-wave method journal, January 1999

Compensation and hydrogen passivation of magnesium acceptors in β-Ga 2 O 3 journal, July 2018

Deep ultraviolet photodiodes based on β-Ga 2 O 3 /SiC heterojunction journal, August 2013

Temperature-dependent exciton resonance energies and their correlation with IR-active optical phonon modes in β-Ga2O3 single crystals journal, March 2016

Valence band ordering in β-Ga 2 O 3 studied by polarized transmittance and reflectance spectroscopy journal, October 2015

Communication—Electrical Characterization of β-Ga 2 O 3 Single Crystal Substrates journal, January 2017

SRIM – The stopping and range of ions in matter (2010) journal, June 2010

Choosing the correct hybrid for defect calculations: A case study on intrinsic carrier trapping in β − G a 2 O 3 journal, February 2017

Experimental electronic structure of In 2 O 3 and Ga 2 O 3 journal, August 2011

Effect of 5 MeV proton irradiation damage on performance of β-Ga 2 O 3 photodetectors journal, July 2016

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

Dielectric properties of electron‐beam deposited Ga 2 O 3 films journal, May 1994

Self-trapped holes in β-Ga 2 O 3 crystals journal, December 2017

A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal, December 2000

Deep-level optical spectroscopy in GaAs journal, May 1981

On the feasibility of p-type Ga 2 O 3 journal, January 2018

Point defect induced degradation of electrical properties of Ga 2 O 3 by 10 MeV proton damage journal, January 2018

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

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

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

Electrical properties of β -Ga 2 O 3 single crystals grown by the Czochralski method journal, September 2011

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

Detailed characterization of deep centers in CdTe: Photoionization and thermal ionization properties journal, January 1982

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

First-principles calculations for defects and impurities: Applications to III-nitrides journal, April 2004

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

Defects responsible for charge carrier removal and correlation with deep level introduction in irradiated β-Ga 2 O 3 journal, August 2018

Electrical conductivity of In 2 O 3 and Ga 2 O 3 after low temperature ion irradiation; implications for instrinsic defect formation and charge neutrality level journal, December 2017

Optical signatures of deep level defects in Ga 2 O 3 journal, June 2018

Density functional tight binding study of β -Ga 2 O 3 : Electronic structure, surface energy, and native point defects journal, May 2019

Influence of the exchange screening parameter on the performance of screened hybrid functionals journal, December 2006

Optical transitions via the deep O donor in GaP. I. Phonon interaction in low-temperature spectra journal, July 1978

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

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

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

First-principles calculations for point defects in solids journal, March 2014

Deep ultraviolet photodiodes based on the β-Ga2O3/GaN heterojunction journal, August 2015

Trapping Effects in Si -Doped -Ga 2 O 3 MESFETs on an Fe-Doped -Ga 2 O 3 Substrate journal, July 2018

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

Photocapacitance effects of deep traps in epitaxial GaAs journal, July 1976

Room-temperature diffusive phenomena in semiconductors: The case of AlGaN journal, December 2011

β-Ga 2 O 3 defect study by steady-state capacitance spectroscopy journal, August 2018

Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces journal, April 2008

Tutorial: Defects in semiconductors—Combining experiment and theory journal, May 2016

Sub-band-gap absorption in Ga 2 O 3 journal, October 2017

Electrical properties of bulk semi-insulating β-Ga 2 O 3 (Fe) journal, October 2018

Formation and annihilation of E4 centers in ZnO: Influence of hydrogen journal, May 2016

Electrostatics-based finite-size corrections for first-principles point defect calculations journal, May 2014

Identification of critical buffer traps in Si δ-doped β-Ga 2 O 3 MESFETs journal, October 2019

Trap Levels in Gallium Arsenide journal, June 1967

Photoionization cross-section analysis for a deep trap contributing to current collapse in GaN field-effect transistors journal, July 2004

Radiation damage effects in Ga 2 O 3 materials and devices journal, January 2019

First-principles theory of acceptors in nitride semiconductors: First-principles theory of acceptors in nitride semiconductors journal, April 2015

On the photoionization of deep impurity centers in semiconductors journal, September 1965

Defect identification based on first-principles calculations for deep level transient spectroscopy journal, November 2018

Compensation and persistent photocapacitance in homoepitaxial Sn-doped β-Ga 2 O 3 journal, March 2018

A combined scanning tunneling microscopy and electron energy loss spectroscopy study on the formation of thin, well-ordered β-Ga2O3 films on CoGa(001) journal, March 1998

Title: Primary intrinsic defects and their charge transition levels in β–Ga₂O₃

Hydrogenated cation vacancies in semiconducting oxides
journal, August 2011

Iron and intrinsic deep level states in Ga ₂ O ₃
journal, January 2018

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

Evolution kinetics of elementary point defects in ZnO implanted with low fluences of helium at cryogenic temperature
journal, November 2016

Projector augmented-wave method
journal, December 1994

Finite-size corrections for defect-involving vertical transitions in supercell calculations
journal, January 2020

Anisotropy, phonon modes, and free charge carrier parameters in monoclinic $β$ -gallium oxide single crystals
journal, March 2016

Deep level defects in Ge-doped (010) β-Ga ₂ O ₃ layers grown by plasma-assisted molecular beam epitaxy
journal, April 2018

Direct Evaluation of Defect Distributions From Admittance Spectroscopy
journal, November 2014

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

A survey of acceptor dopants for β -Ga ₂ O ₃
journal, April 2018

Optical evidence of intrinsic quantum wells in the transparent conducting oxide β-Ga2O3
journal, August 2000

Hole traps and persistent photocapacitance in proton irradiated β-Ga ₂ O ₃ films doped with Si
journal, September 2018

Fully Ab Initio Finite-Size Corrections for Charged-Defect Supercell Calculations
journal, January 2009

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Compensation and hydrogen passivation of magnesium acceptors in β-Ga ₂ O ₃
journal, July 2018

Deep ultraviolet photodiodes based on β-Ga ₂ O ₃ /SiC heterojunction
journal, August 2013

Temperature-dependent exciton resonance energies and their correlation with IR-active optical phonon modes in β-Ga2O3 single crystals
journal, March 2016

Valence band ordering in β-Ga ₂ O ₃ studied by polarized transmittance and reflectance spectroscopy
journal, October 2015

Communication—Electrical Characterization of β-Ga ₂ O ₃ Single Crystal Substrates
journal, January 2017

SRIM – The stopping and range of ions in matter (2010)
journal, June 2010

Choosing the correct hybrid for defect calculations: A case study on intrinsic carrier trapping in $β - G a_{2} O_{3}$
journal, February 2017

Experimental electronic structure of In ₂ O ₃ and Ga ₂ O ₃
journal, August 2011

Effect of 5 MeV proton irradiation damage on performance of β-Ga ₂ O ₃ photodetectors
journal, July 2016

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

Dielectric properties of electron‐beam deposited Ga ₂ O ₃ films
journal, May 1994

Self-trapped holes in β-Ga ₂ O ₃ crystals
journal, December 2017

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

Deep-level optical spectroscopy in GaAs
journal, May 1981

On the feasibility of p-type Ga ₂ O ₃
journal, January 2018

Point defect induced degradation of electrical properties of Ga ₂ O ₃ by 10 MeV proton damage
journal, January 2018

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

Migration mechanisms and diffusion barriers of vacancies in ${Ga}_{2} O_{3}$
journal, June 2017

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

Electrical properties of β -Ga ₂ O ₃ single crystals grown by the Czochralski method
journal, September 2011

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

Detailed characterization of deep centers in CdTe: Photoionization and thermal ionization properties
journal, January 1982

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

First-principles calculations for defects and impurities: Applications to III-nitrides
journal, April 2004

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

Defects responsible for charge carrier removal and correlation with deep level introduction in irradiated β-Ga ₂ O ₃
journal, August 2018

Electrical conductivity of In ₂ O ₃ and Ga ₂ O ₃ after low temperature ion irradiation; implications for instrinsic defect formation and charge neutrality level
journal, December 2017

Optical signatures of deep level defects in Ga ₂ O ₃
journal, June 2018

Density functional tight binding study of β -Ga ₂ O ₃ : Electronic structure, surface energy, and native point defects
journal, May 2019

Influence of the exchange screening parameter on the performance of screened hybrid functionals
journal, December 2006

Optical transitions via the deep O donor in GaP. I. Phonon interaction in low-temperature spectra
journal, July 1978

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

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

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

First-principles calculations for point defects in solids
journal, March 2014

Deep ultraviolet photodiodes based on the β-Ga2O3/GaN heterojunction
journal, August 2015

Trapping Effects in Si -Doped -Ga ₂ O ₃ MESFETs on an Fe-Doped -Ga ₂ O ₃ Substrate
journal, July 2018

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

Photocapacitance effects of deep traps in epitaxial GaAs
journal, July 1976

Room-temperature diffusive phenomena in semiconductors: The case of AlGaN
journal, December 2011

β-Ga ₂ O ₃ defect study by steady-state capacitance spectroscopy
journal, August 2018

Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces
journal, April 2008

Tutorial: Defects in semiconductors—Combining experiment and theory
journal, May 2016

Sub-band-gap absorption in Ga ₂ O ₃
journal, October 2017

Electrical properties of bulk semi-insulating β-Ga ₂ O ₃ (Fe)
journal, October 2018

Formation and annihilation of E4 centers in ZnO: Influence of hydrogen
journal, May 2016

Electrostatics-based finite-size corrections for first-principles point defect calculations
journal, May 2014

Identification of critical buffer traps in Si δ-doped β-Ga ₂ O ₃ MESFETs
journal, October 2019

Trap Levels in Gallium Arsenide
journal, June 1967

Photoionization cross-section analysis for a deep trap contributing to current collapse in GaN field-effect transistors
journal, July 2004

Radiation damage effects in Ga ₂ O ₃ materials and devices
journal, January 2019

First-principles theory of acceptors in nitride semiconductors: First-principles theory of acceptors in nitride semiconductors
journal, April 2015

On the photoionization of deep impurity centers in semiconductors
journal, September 1965

Defect identification based on first-principles calculations for deep level transient spectroscopy
journal, November 2018

Compensation and persistent photocapacitance in homoepitaxial Sn-doped β-Ga ₂ O ₃
journal, March 2018

A combined scanning tunneling microscopy and electron energy loss spectroscopy study on the formation of thin, well-ordered β-Ga2O3 films on CoGa(001)
journal, March 1998