Direct Observation of Sr Vacancies in SrTiO 3 by Quantitative Scanning Transmission Electron Microscopy

Kim, Honggyu; Zhang, Jack Y.; Raghavan, Santosh; Stemmer, Susanne

doi:10.1103/PhysRevX.6.041063

Title: Direct Observation of Sr Vacancies in ${SrTiO}_{3}$ by Quantitative Scanning Transmission Electron Microscopy

Abstract

Unveiling the identity, spatial configuration, and microscopic structure of point defects is one of the key challenges in materials science. Here, we demonstrate that quantitative scanning transmission electron microscopy (STEM) can be used to directly observe Sr vacancies in SrTiO₃ and to determine the atom column relaxations around them. By combining recent advances in quantitative STEM, including variableangle, high-angle annular dark-field imaging and rigid registration methods, with frozen phonon multislice image simulations, we identify which Sr columns contain vacancies and quantify the number of vacancies in them. Here, picometer precision measurements of the surrounding atom column positions show that the nearest-neighbor Ti atoms are displaced away from the Sr vacancies. The results open up a new methodology for studying the microscopic mechanisms by which point defects control materials properties.

Authors:: Kim, Honggyu; Zhang, Jack Y.; Raghavan, Santosh; Stemmer, Susanne

Publication Date:: Thu Dec 22 00:00:00 EST 2016

Research Org.:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1337451

Alternate Identifier(s):: OSTI ID: 1361394

Grant/Contract Number:: FG02-02ER45994

Resource Type:: Published Article

Journal Name:: Physical Review. X

Additional Journal Information:: Journal Name: Physical Review. X Journal Volume: 6 Journal Issue: 4; Journal ID: ISSN 2160-3308

Publisher:: American Physical Society

Country of Publication:: United States

Language:: English

Subject:: 74 ATOMIC AND MOLECULAR PHYSICS; 36 MATERIALS SCIENCE

Citation Formats


                    Kim, Honggyu, Zhang, Jack Y., Raghavan, Santosh, and Stemmer, Susanne. Direct Observation of Sr Vacancies in SrTiO 3 by Quantitative Scanning Transmission Electron Microscopy.  United States: N. p., 2016. 
Web.  doi:10.1103/PhysRevX.6.041063.

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                    Kim, Honggyu, Zhang, Jack Y., Raghavan, Santosh, & Stemmer, Susanne. Direct Observation of Sr Vacancies in SrTiO 3 by Quantitative Scanning Transmission Electron Microscopy.  United States.  https://doi.org/10.1103/PhysRevX.6.041063

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                    Kim, Honggyu, Zhang, Jack Y., Raghavan, Santosh, and Stemmer, Susanne. Thu .  
"Direct Observation of Sr Vacancies in SrTiO 3 by Quantitative Scanning Transmission Electron Microscopy".  United States.  https://doi.org/10.1103/PhysRevX.6.041063.

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@article{osti_1337451,

  title        = {Direct Observation of Sr Vacancies in SrTiO 3 by Quantitative Scanning Transmission Electron Microscopy},

  author       = {Kim, Honggyu and Zhang, Jack Y. and Raghavan, Santosh and Stemmer, Susanne},

  abstractNote = {Unveiling the identity, spatial configuration, and microscopic structure of point defects is one of the key challenges in materials science. Here, we demonstrate that quantitative scanning transmission electron microscopy (STEM) can be used to directly observe Sr vacancies in SrTiO3 and to determine the atom column relaxations around them. By combining recent advances in quantitative STEM, including variableangle, high-angle annular dark-field imaging and rigid registration methods, with frozen phonon multislice image simulations, we identify which Sr columns contain vacancies and quantify the number of vacancies in them. Here, picometer precision measurements of the surrounding atom column positions show that the nearest-neighbor Ti atoms are displaced away from the Sr vacancies. The results open up a new methodology for studying the microscopic mechanisms by which point defects control materials properties.},

  doi          = {10.1103/PhysRevX.6.041063},

  journal      = {Physical Review. X},

  number       = 4,

  volume       = 6,

  place        = {United States},

  year         = {Thu Dec 22 00:00:00 EST 2016},

  month        = {Thu Dec 22 00:00:00 EST 2016}

}

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Title: Direct Observation of Sr Vacancies in SrTiO 3 by Quantitative Scanning Transmission Electron Microscopy

Abstract

Citation Formats

Three-Dimensional Location of a Single Dopant with Atomic Precision by Aberration-Corrected Scanning Transmission Electron Microscopy journal, March 2014

Surface reconstructions in molecular beam epitaxy of SrTiO 3 journal, November 2014

Revolving scanning transmission electron microscopy: Correcting sample drift distortion without prior knowledge journal, March 2014

Defects in Semiconductors: Some Fatal, Some Vital journal, August 1998

Electron Correlation in Oxygen Vacancy in SrTiO 3 journal, November 2013

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

Growth of homoepitaxial SrTiO3 thin films by molecular-beam epitaxy journal, April 2009

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Emergence of room-temperature ferroelectricity at reduced dimensions journal, September 2015

Strontium vacancy clustering in Ti-excess SrTiO 3 thin film journal, July 2011

Advanced Computing in Electron Microscopy book, January 2010

Vacancies and small polarons in SrTiO 3 journal, August 2014

Elastic effects of vacancies in strontium titanate: Short- and long-range strain fields, elastic dipole tensors, and chemical strain journal, August 2009

LaAlO3 stoichiometry is key to electron liquid formation at LaAlO3/SrTiO3 interfaces journal, August 2013

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Insulating Ferromagnetic LaCoO 3 − δ Films: A Phase Induced by Ordering of Oxygen Vacancies journal, February 2014

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Dramatic mobility enhancements in doped SrTiO3 thin films by defect management journal, July 2010

Variable-angle high-angle annular dark-field imaging: application to three-dimensional dopant atom profiling journal, July 2015

Growth of high-quality SrTiO3 films using a hybrid molecular beam epitaxy approach journal, May 2009

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Ferroelectricity in Strain-Free SrTiO 3 Thin Films journal, May 2010

First-principles study on structures and energetics of intrinsic vacancies in SrTiO 3 journal, November 2003

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

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Doping a Mott insulator: Physics of high-temperature superconductivity journal, January 2006

Deep donor levels ( D X centers) in III‐V semiconductors journal, February 1990

Defects and transport in complex oxide thin films journal, May 2008

Computer Simulation Studies of Strontium Titanate journal, February 1995

Role of Ti Antisitelike Defects in SrTiO 3 journal, October 2009

Nonstoichiometry in SrTiO[sub 3] journal, January 1981

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

Point Defect Configurations of Supersaturated Au Atoms Inside Si Nanowires journal, March 2008

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

Probing oxygen vacancy concentration and homogeneity in solid-oxide fuel-cell cathode materials on the subunit-cell level journal, August 2012

Title: Direct Observation of Sr Vacancies in ${SrTiO}_{3}$ by Quantitative Scanning Transmission Electron Microscopy

Three-Dimensional Location of a Single Dopant with Atomic Precision by Aberration-Corrected Scanning Transmission Electron Microscopy
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Surface reconstructions in molecular beam epitaxy of SrTiO ₃
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Revolving scanning transmission electron microscopy: Correcting sample drift distortion without prior knowledge
journal, March 2014

Defects in Semiconductors: Some Fatal, Some Vital
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Electron Correlation in Oxygen Vacancy in ${SrTiO}_{3}$
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Atomic-scale imaging of nanoengineered oxygen vacancy profiles in SrTiO3
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Growth of homoepitaxial SrTiO3 thin films by molecular-beam epitaxy
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journal, August 2013

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journal, June 2014

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journal, October 2013

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journal, July 2010

Variable-angle high-angle annular dark-field imaging: application to three-dimensional dopant atom profiling
journal, July 2015

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journal, July 2011

Disorder-driven non-Fermi liquid behaviour of correlated electrons
journal, August 2005

Ferroelectricity in Strain-Free ${SrTiO}_{3}$ Thin Films
journal, May 2010

First-principles study on structures and energetics of intrinsic vacancies in ${SrTiO}_{3}$
journal, November 2003

The Metal-Insulator Transition in Correlated Disordered Systems
journal, December 1996

Defect structure in homoepitaxial non-stoichiometric strontium titanate thin films
journal, March 2000

Quantitative Atomic Resolution Scanning Transmission Electron Microscopy
journal, May 2008

Three-Dimensional Imaging of Individual Dopant Atoms in ${SrTiO}_{3}$
journal, December 2013

Impact of stress on oxygen vacancy ordering in epitaxial (La0.5Sr0.5)CoO3−∂ thin films
journal, May 2003

Optimal ADF STEM imaging parameters for tilt-robust image quantification
journal, September 2015

Perspective: Oxide molecular-beam epitaxy rocks!
journal, June 2015

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

Doping a Mott insulator: Physics of high-temperature superconductivity
journal, January 2006

Deep donor levels ( D X centers) in III‐V semiconductors
journal, February 1990

Defects and transport in complex oxide thin films
journal, May 2008

Computer Simulation Studies of Strontium Titanate
journal, February 1995

Role of Ti Antisitelike Defects in ${SrTiO}_{3}$
journal, October 2009

Nonstoichiometry in SrTiO[sub 3]
journal, January 1981

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

Point Defect Configurations of Supersaturated Au Atoms Inside Si Nanowires
journal, March 2008

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

Probing oxygen vacancy concentration and homogeneity in solid-oxide fuel-cell cathode materials on the subunit-cell level
journal, August 2012