Isolated oxygen vacancies in strontium titanate shine red: Optical identification of Ti3+ polarons

Crespillo, M. L.; Graham, J. T.; Agulló-López, F.; Zhang, Y.; Weber, W. J.

doi:10.1016/j.apmt.2018.04.006

Title: Isolated oxygen vacancies in strontium titanate shine red: Optical identification of Ti³⁺ polarons

Abstract

Oxide perovskites exhibit fascinating physical properties that identify them as key materials for the next generation of oxide-based functional electronic devices, as well as for catalysis and photochemistry applications. In strontium titanate, substantial efforts have been devoted to elucidate the role of oxygen vacancies and localized electronic states, such as polarons, on those properties. In this paper, a new model is presented that assigns a definitive red luminescence signature at 2.0 eV to Ti³⁺ polarons trapped at isolated oxygen vacancies. This emission provides an unequivocal identification for the oxygen vacancies, which allows monitoring their creation and annealing by a variety of physio-chemical treatments. Ionoluminescence with energetic (MeV) ion beams enables such identification by combining the sensitivity and resolution of spectroscopic techniques with their in situ character, as well as controlled incorporation of point defects, such as oxygen vacancies. Alternative models assigning the blue luminescence emission at 2.8 eV to oxygen vacancies are not supported by the experimental results. Finally and therefore, oxygen vacancies shine red and not blue, as previously proposed.

Authors:

Crespillo, M. L. ^[1]; Graham, J. T. ^[2]; Agulló-López, F. ^[3]; Zhang, Y. ^[4];

^[5]

Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
Missouri Univ. of Science and Technology, Rolla, MO (United States). Dept. of Mining and Nuclear Engineering; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
Autonomous Univ. of Madrid (Spain). Centre for the Micro Analysis of Materials (CMAM)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division

Publication Date:: Thu Aug 30 00:00:00 EDT 2018

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Univ. of Tennessee (United States)

OSTI Identifier:: 1468192

Alternate Identifier(s):: OSTI ID: 1698193

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Applied Materials Today

Additional Journal Information:: Journal Volume: 12; Journal ID: ISSN 2352-9407

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; strontium titanate; defects; oxygen vacancies; polarons; ionoluminescence

Citation Formats


                    Crespillo, M. L., Graham, J. T., Agulló-López, F., Zhang, Y., and Weber, W. J. Isolated oxygen vacancies in strontium titanate shine red: Optical identification of Ti3+ polarons.  United States: N. p., 2018. 
Web.  doi:10.1016/j.apmt.2018.04.006.

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                    Crespillo, M. L., Graham, J. T., Agulló-López, F., Zhang, Y., & Weber, W. J. Isolated oxygen vacancies in strontium titanate shine red: Optical identification of Ti3+ polarons.  United States.  https://doi.org/10.1016/j.apmt.2018.04.006

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                    Crespillo, M. L., Graham, J. T., Agulló-López, F., Zhang, Y., and Weber, W. J. Thu .  
"Isolated oxygen vacancies in strontium titanate shine red: Optical identification of Ti3+ polarons".  United States.  https://doi.org/10.1016/j.apmt.2018.04.006.  https://www.osti.gov/servlets/purl/1468192.

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@article{osti_1468192,

  title        = {Isolated oxygen vacancies in strontium titanate shine red: Optical identification of Ti3+ polarons},

  author       = {Crespillo, M. L. and Graham, J. T. and Agulló-López, F. and Zhang, Y. and Weber, W. J.},

  abstractNote = {Oxide perovskites exhibit fascinating physical properties that identify them as key materials for the next generation of oxide-based functional electronic devices, as well as for catalysis and photochemistry applications. In strontium titanate, substantial efforts have been devoted to elucidate the role of oxygen vacancies and localized electronic states, such as polarons, on those properties. In this paper, a new model is presented that assigns a definitive red luminescence signature at 2.0 eV to Ti3+ polarons trapped at isolated oxygen vacancies. This emission provides an unequivocal identification for the oxygen vacancies, which allows monitoring their creation and annealing by a variety of physio-chemical treatments. Ionoluminescence with energetic (MeV) ion beams enables such identification by combining the sensitivity and resolution of spectroscopic techniques with their in situ character, as well as controlled incorporation of point defects, such as oxygen vacancies. Alternative models assigning the blue luminescence emission at 2.8 eV to oxygen vacancies are not supported by the experimental results. Finally and therefore, oxygen vacancies shine red and not blue, as previously proposed.},

  doi          = {10.1016/j.apmt.2018.04.006},

  journal      = {Applied Materials Today},

  number       = ,

  volume       = 12,

  place        = {United States},

  year         = {Thu Aug 30 00:00:00 EDT 2018},

  month        = {Thu Aug 30 00:00:00 EDT 2018}

}

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https://doi.org/10.1016/j.apmt.2018.04.006

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Works referencing / citing this record:

The blue emission at 2.8 eV in strontium titanate: evidence for a radiative transition of self-trapped excitons from unbound states
journal, April 2019

Crespillo, M. L.; Graham, J. T.; Agulló-López, F.
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Resistance Switching Behavior in Rectangle-Nano-Pattern SrTiO3 Induced by Simple Annealing
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Liao, Xiaxia; Zhang, Yufeng; Wang, Jiaou
Materials, Vol. 12, Issue 22
DOI: 10.3390/ma12223698

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Title: Isolated oxygen vacancies in strontium titanate shine red: Optical identification of Ti3+ polarons

Abstract

Citation Formats

Superconducting Interfaces Between Insulating Oxides journal, August 2007

Magnetic effects at the interface between non-magnetic oxides journal, June 2007

Photophysical and Photocatalytic Properties of SrTiO 3 Doped with Cr Cations on Different Sites journal, August 2006

Tunable Electronic Structure and Surface Defects in Chromium-Doped Colloidal SrTiO 3−δ Nanocrystals journal, January 2016

Blue-light emission at room temperature from Ar+-irradiated SrTiO3 journal, October 2005

Oxygen vacancies shine blue journal, November 2005

Recombination kinetics of a dense electron-hole plasma in strontium titanate journal, September 2007

Temperature Dependence of Photoluminescence Spectra of Nondoped and Electron-Doped SrTiO 3 : Crossover from Auger Recombination to Single-Carrier Trapping journal, June 2009

Vacancies and small polarons in SrTiO 3 journal, August 2014

Role of oxygen vacancies on light emission mechanisms in SrTiO 3 induced by high-energy particles journal, March 2017

Correlation between Cr 3+ Luminescence and Oxygen Vacancy Disorder in Strontium Titanate under MeV Ion Irradiation journal, September 2017

Electronic structure of a neutral oxygen vacancy in SrTiO 3 journal, December 2003

Defect States Induced by Oxygen Vacancies in Cubic SrTiO 3 : First-Principles Calculations journal, November 2010

Electronic structure of oxygen vacancies in SrTiO 3 and LaAlO 3 journal, October 2012

First-principles study of bulk and surface oxygen vacancies in SrTiO3 crystal journal, October 2009

Anti-ferrodistortive-Like Oxygen-Octahedron Rotation Induced by the Oxygen Vacancy in Cubic SrTiO 3 journal, October 2012

Structural and electronic properties of n -doped and p -doped Sr Ti O 3 journal, December 2004

Structural and electronic properties of oxygen vacancies in cubic and antiferrodistortive phases of SrTiO 3 journal, May 2004

Symmetry-breaking Ta 4 + centers in KTaO 3 journal, July 1998

Atomic-scale control of TiO6 octahedra through solution chemistry towards giant dielectric response journal, October 2014

Spectra and color centers of strontium titanate crystals journal, January 2012

Room-temperature photoluminescence in amorphous SrTiO 3 - the influence of acceptor-type dopants journal, November 2002

In-Gap States in Wide-Band-Gap SrTiO3 Analyzed by Cathodoluminescence: In-Gap States in Wide-Band-Gap SrTiO3 journal, March 2011

X‐ray induced processes in SrTiO 3 journal, December 1982

New ion beam materials laboratory for materials modification and irradiation effects research journal, November 2014

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

Model of ion-induced luminescence based on energy deposition by secondary electrons journal, June 1994

Hole localization, migration, and the formation of peroxide anion in perovskite Sr Ti O 3 journal, July 2014

Temperature measurements during high flux ion beam irradiations journal, February 2016

Charge-Carrier Transport Phenomena in Amorphous Si O 2 : Direct Measurement of the Drift Mobility and Lifetime journal, June 1973

Semiconductor Radiation Detectors: Basic principles and some uses of a recent tool that has revolutionized nuclear physics are described journal, October 1970

In-situ luminescence monitoring of ion-induced damage evolution in SiO2 and Al2O3 journal, April 2016

The blue emission at 2.8 eV in strontium titanate: evidence for a radiative transition of self-trapped excitons from unbound states journal, April 2019

Resistance Switching Behavior in Rectangle-Nano-Pattern SrTiO3 Induced by Simple Annealing journal, November 2019

Title: Isolated oxygen vacancies in strontium titanate shine red: Optical identification of Ti³⁺ polarons

Superconducting Interfaces Between Insulating Oxides
journal, August 2007

Magnetic effects at the interface between non-magnetic oxides
journal, June 2007

Photophysical and Photocatalytic Properties of SrTiO ₃ Doped with Cr Cations on Different Sites
journal, August 2006

Tunable Electronic Structure and Surface Defects in Chromium-Doped Colloidal SrTiO _3−δ Nanocrystals
journal, January 2016

Blue-light emission at room temperature from Ar+-irradiated SrTiO3
journal, October 2005

Oxygen vacancies shine blue
journal, November 2005

Recombination kinetics of a dense electron-hole plasma in strontium titanate
journal, September 2007

Temperature Dependence of Photoluminescence Spectra of Nondoped and Electron-Doped ${SrTiO}_{3}$ : Crossover from Auger Recombination to Single-Carrier Trapping
journal, June 2009

Vacancies and small polarons in ${SrTiO}_{3}$
journal, August 2014

Role of oxygen vacancies on light emission mechanisms in SrTiO ₃ induced by high-energy particles
journal, March 2017

Correlation between Cr ³⁺ Luminescence and Oxygen Vacancy Disorder in Strontium Titanate under MeV Ion Irradiation
journal, September 2017

Electronic structure of a neutral oxygen vacancy in ${SrTiO}_{3}$
journal, December 2003

Defect States Induced by Oxygen Vacancies in Cubic SrTiO ₃ : First-Principles Calculations
journal, November 2010

Electronic structure of oxygen vacancies in ${SrTiO}_{3}$ and ${LaAlO}_{3}$
journal, October 2012

First-principles study of bulk and surface oxygen vacancies in SrTiO3 crystal
journal, October 2009

Anti-ferrodistortive-Like Oxygen-Octahedron Rotation Induced by the Oxygen Vacancy in Cubic SrTiO ₃
journal, October 2012

Structural and electronic properties of $n$ -doped and $p$ -doped $Sr Ti O_{3}$
journal, December 2004

Structural and electronic properties of oxygen vacancies in cubic and antiferrodistortive phases of ${SrTiO}_{3}$
journal, May 2004

Symmetry-breaking ${Ta}^{4 +}$ centers in ${KTaO}_{3}$
journal, July 1998

Atomic-scale control of TiO6 octahedra through solution chemistry towards giant dielectric response
journal, October 2014

Spectra and color centers of strontium titanate crystals
journal, January 2012

Room-temperature photoluminescence in amorphous SrTiO 3 - the influence of acceptor-type dopants
journal, November 2002

In-Gap States in Wide-Band-Gap SrTiO3 Analyzed by Cathodoluminescence: In-Gap States in Wide-Band-Gap SrTiO3
journal, March 2011

X‐ray induced processes in SrTiO ₃
journal, December 1982

New ion beam materials laboratory for materials modification and irradiation effects research
journal, November 2014

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

Model of ion-induced luminescence based on energy deposition by secondary electrons
journal, June 1994

Hole localization, migration, and the formation of peroxide anion in perovskite ${Sr Ti O}_{3}$
journal, July 2014

Temperature measurements during high flux ion beam irradiations
journal, February 2016

Charge-Carrier Transport Phenomena in Amorphous Si $O_{2}$ : Direct Measurement of the Drift Mobility and Lifetime
journal, June 1973

Semiconductor Radiation Detectors: Basic principles and some uses of a recent tool that has revolutionized nuclear physics are described
journal, October 1970

In-situ luminescence monitoring of ion-induced damage evolution in SiO2 and Al2O3
journal, April 2016

The blue emission at 2.8 eV in strontium titanate: evidence for a radiative transition of self-trapped excitons from unbound states
journal, April 2019

Resistance Switching Behavior in Rectangle-Nano-Pattern SrTiO3 Induced by Simple Annealing
journal, November 2019