How heteroepitaxy occurs on strontium titanate

Cook, Seyoung; Letchworth-Weaver, Kendra; Tung, I-Cheng; Andersen, Tassie K.; Hong, Hawoong; Marks, Laurence D.; Fong, Dillon D.

doi:10.1126/sciadv.aav0764

Title: How heteroepitaxy occurs on strontium titanate

Abstract

In traditional models of heteroepitaxy, the substrate serves mainly as a crystalline template for the thin-film lattice, dictating the initial roughness of the film and the degree of coherent strain. Here, performing in situ surface x-ray diffraction during the heteroepitaxial growth of LaTiO₃on SrTiO₃(001), we find that a TiO₂adlayer composed of the $(\sqrt{13} \times \sqrt{13})$ R33.7° and $(\sqrt{2} \times \sqrt{2})$ R45.0° reconstructions is a highly active participant in the growth process, continually diffusing to the surface throughout deposition. The effects of the TiO₂adlayer on layer-by-layer growth are investigated using different deposition sequences and anomalous x-ray scattering, both of which permit detailed insight into the dynamic layer rearrangements that take place. Our work challenges commonly held assumptions regarding growth on TiO₂-terminated SrTiO₃(001) and demonstrates the critical role of excess TiO₂surface stoichiometry on the initial stages of heteroepitaxial growth on this important perovskite oxide substrate material.

Authors:

^[1]; Letchworth-Weaver, Kendra ^[2];

^[3];

^[1];

^[3]; Marks, Laurence D. ^[4];

^[3]

Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); James Madison Univ., Harrisonburg, VA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Northwestern Univ., Evanston, IL (United States)

Publication Date:: Fri Apr 12 00:00:00 EDT 2019

Research Org.:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1524409

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Science Advances

Additional Journal Information:: Journal Volume: 5; Journal Issue: 4; Journal ID: ISSN 2375-2548

Publisher:: AAAS

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Cook, Seyoung, Letchworth-Weaver, Kendra, Tung, I-Cheng, Andersen, Tassie K., Hong, Hawoong, Marks, Laurence D., and Fong, Dillon D. How heteroepitaxy occurs on strontium titanate.  United States: N. p., 2019. 
Web.  doi:10.1126/sciadv.aav0764.

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                    Cook, Seyoung, Letchworth-Weaver, Kendra, Tung, I-Cheng, Andersen, Tassie K., Hong, Hawoong, Marks, Laurence D., & Fong, Dillon D. How heteroepitaxy occurs on strontium titanate.  United States.  https://doi.org/10.1126/sciadv.aav0764

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                    Cook, Seyoung, Letchworth-Weaver, Kendra, Tung, I-Cheng, Andersen, Tassie K., Hong, Hawoong, Marks, Laurence D., and Fong, Dillon D. Fri .  
"How heteroepitaxy occurs on strontium titanate".  United States.  https://doi.org/10.1126/sciadv.aav0764.  https://www.osti.gov/servlets/purl/1524409.

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@article{osti_1524409,

  title        = {How heteroepitaxy occurs on strontium titanate},

  author       = {Cook, Seyoung and Letchworth-Weaver, Kendra and Tung, I-Cheng and Andersen, Tassie K. and Hong, Hawoong and Marks, Laurence D. and Fong, Dillon D.},

  abstractNote = {In traditional models of heteroepitaxy, the substrate serves mainly as a crystalline template for the thin-film lattice, dictating the initial roughness of the film and the degree of coherent strain. Here, performing in situ surface x-ray diffraction during the heteroepitaxial growth of LaTiO3on SrTiO3(001), we find that a TiO2adlayer composed of the(13×13)R33.7° and(2×2)R45.0° reconstructions is a highly active participant in the growth process, continually diffusing to the surface throughout deposition. The effects of the TiO2adlayer on layer-by-layer growth are investigated using different deposition sequences and anomalous x-ray scattering, both of which permit detailed insight into the dynamic layer rearrangements that take place. Our work challenges commonly held assumptions regarding growth on TiO2-terminated SrTiO3(001) and demonstrates the critical role of excess TiO2surface stoichiometry on the initial stages of heteroepitaxial growth on this important perovskite oxide substrate material.},

  doi          = {10.1126/sciadv.aav0764},

  journal      = {Science Advances},

  number       = 4,

  volume       = 5,

  place        = {United States},

  year         = {Fri Apr 12 00:00:00 EDT 2019},

  month        = {Fri Apr 12 00:00:00 EDT 2019}

}

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FIG. 1: (a) Bare SrTiO₃ (001) surface after following the standard etch-and-anneal procedure, exhibiting ~0.4nm high steps with both ( $\sqrt{13}$ x $\sqrt{13}$)$R$33.7° (RT13) and ( $\sqrt{2}$ x $\sqrt{2}$)$R$45.0° (RT2) surface reconstructions. (b) Schematic of LaTiO₃ growth by oxide MBE following either the TiO₂/LaO (T/L) or LaO/TiO₂ (L/T) growth sequencemore »

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Title: How heteroepitaxy occurs on strontium titanate

Abstract

Citation Formats

Figures / Tables:

Epitaxial Growth Process of La 0.7 Ca 0.3 MnO 3 Thin Films on SrTiO 3 (001): Thickness-Dependent Inhomogeneity Caused by Excess Ti Atoms journal, March 2014

A Single-Atom-Thick TiO 2 Nanomesh on an Insulating Oxide journal, August 2015

Structure of the Photo-catalytically Active Surface of SrTiO 3 journal, June 2016

Interface-induced superconductivity and strain-dependent spin density waves in FeSe/SrTiO3 thin films journal, May 2013

Surface Structures of SrTiO 3 (001): A TiO 2 -rich Reconstruction with a c(4 × 2) Unit Cell journal, August 2003

Two-Dimensional Superconducting Phase in LaTiO 3 / SrTiO 3 Heterostructures Induced by High-Mobility Carrier Doping journal, June 2012

Metallic and Insulating Oxide Interfaces Controlled by Electronic Correlations journal, February 2011

Two-Dimensional Electron Gases at Complex Oxide Interfaces journal, July 2014

Superconductivity above 100 K in single-layer FeSe films on doped SrTiO3 journal, November 2014

Filling dependence of electronic properties on the verge of metal–Mott-insulator transition in Sr 1 − x La x TiO 3 journal, April 1993

Atomically precise interfaces from non-stoichiometric deposition journal, August 2014

Atomic-Scale Visualization of Initial Growth of Homoepitaxial SrTiO 3 Thin Film on an Atomically Ordered Substrate journal, September 2011

The structure and chemistry of the TiO2-rich surface of SrTiO3 (001) journal, September 2002

Realization of atomically flat steps and terraces like surface of SrTiO3 (001) single crystal by hot water etching and high temperature annealing journal, July 2015

Elastic Constants of Strontium Titanate journal, January 1963

Quantum many-body interactions in digital oxide superlattices journal, August 2012

X-Ray Scattering Studies of the Surface Structure of Complex Oxide Films during Layer-by-Layer Growth via Pulsed Laser Deposition journal, July 2009

Surfactant-mediated molecular beam epitaxy of strained layer semiconductor heterostructures journal, August 1993

Atomic control and characterization of surface defect states of TiO2 terminated SrTiO3 single crystals journal, August 2008

Universal Ti-rich termination of atomically flat SrTiO3 (001), (110), and (111) surfaces journal, January 2011

Vapor deposition processes for amorphous carbon films with sp 3 fractions approaching diamond journal, August 1991

Atomic Control of the SrTiO3 Crystal Surface journal, December 1994

Correlated Oxide Physics and Electronics journal, July 2014

Nucleation, coarsening, and coalescence during layer-by-layer growth of complex oxides via pulsed laser deposition: Time-resolved, diffuse X-ray scattering studies journal, November 2010

Two-dimensional superconductivity at a Mott insulator/band insulator interface LaTiO3/SrTiO3 journal, October 2010

Surface transmission electron diffraction for SrTiO3 surfaces journal, January 2012

High mobility conduction at (110) and (111) LaAlO3/SrTiO3 interfaces journal, October 2012

A Thin Film Approach to Engineering Functionality into Oxides journal, August 2008

Surface determination through atomically resolved secondary-electron imaging journal, June 2015

In situ surface/interface x-ray diffractometer for oxide molecular beam epitaxy journal, January 2016

Experimental verification of the phonon dispersion curves of strontium titanate journal, October 1976

Epitaxial growth and electronic structure of LaTiOx films journal, May 2002

Mechanisms of charge transfer and redistribution in LaAlO3/SrTiO3 revealed by high-energy optical conductivity journal, April 2014

TiO2-rich reconstructions of SrTiO3(001): a theoretical study of structural patterns journal, December 2004

Multiband superconductivity and nanoscale inhomogeneity at oxide interfaces journal, July 2013

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

Ab Initio Predictions of Double-Layer TiO 2 -Terminated SrTiO 3 (001) Surface Reconstructions journal, August 2018

Transport in ferromagnetic GdTiO3/SrTiO3 heterostructures journal, March 2011

Measurements of Surface Diffusivity and Coarsening during Pulsed Laser Deposition journal, December 2009

Emergent phenomena at oxide interfaces journal, January 2012

A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface journal, January 2004

Tunable Quasi-Two-Dimensional Electron Gases in Oxide Heterostructures journal, September 2006

Characterization of the X-ray coherence properties of an undulator beamline at the Advanced Photon Source journal, June 2018

Metallic and Insulating Interfaces of Amorphous SrTiO 3 -Based Oxide Heterostructures journal, September 2011

Superconducting Interfaces Between Insulating Oxides journal, August 2007

The (2×2) reconstructions on the SrTiO3 (001) surface: A combined scanning tunneling microscopy and density functional theory study journal, September 2011

Direct observation of a two-dimensional hole gas at oxide interfaces journal, February 2018

Photoemission from Buried Interfaces in SrTiO 3 / LaTiO 3 Superlattices journal, August 2006

Crystal truncation rods from miscut surfaces journal, May 2017

Artificial charge-modulationin atomic-scale perovskite titanate superlattices journal, September 2002

A high-mobility two-dimensional electron gas at the spinel/perovskite interface of γ-Al2O3/SrTiO3 journal, January 2013

Vacant-Site Octahedral Tilings on SrTiO 3 (001), the ( 13 × 13 ) R 33.7 ° Surface, and Related Structures journal, April 2011

Quasi-ideal strontium titanate crystal surfaces through formation of strontium hydroxide journal, November 1998

Layer-by-Layer Evolution of a Two-Dimensional Electron Gas Near an Oxide Interface journal, September 2013

Interfacial dielectric layer as an origin of polarization fatigue in ferroelectric capacitors journal, April 2020

Measurements of Surface Diffusivity and Coarsening During Pulsed Laser Deposition text, January 2009

Multi-band superconductivity and nanoscale inhomogeneity at oxide interfaces text, January 2013

Crystal truncation rods from miscut surfaces text, January 2017

A Single-Atom-Thick TiO 2 Nanomesh on an Insulating Oxide journal, August 2015

Epitaxial Growth Process of La 0.7 Ca 0.3 MnO 3 Thin Films on SrTiO 3 (001): Thickness-Dependent Inhomogeneity Caused by Excess Ti Atoms journal, March 2014

Surface Structures of SrTiO 3 (001): A TiO 2 -rich Reconstruction with a c(4 × 2) Unit Cell journal, August 2003

Structure of the Photo-catalytically Active Surface of SrTiO 3 journal, June 2016

Edge effects journal, September 2002

Artificial charge-modulationin atomic-scale perovskite titanate superlattices journal, September 2002

Two-dimensional superconductivity at a Mott insulator/band insulator interface LaTiO3/SrTiO3 journal, October 2010

A high-mobility two-dimensional electron gas at the spinel/perovskite interface of γ-Al2O3/SrTiO3 journal, January 2013

Emergent phenomena at oxide interfaces journal, January 2012

Superconductivity above 100 K in single-layer FeSe films on doped SrTiO3 journal, November 2014

2D hole gas seen journal, February 2018

Quasi-ideal strontium titanate crystal surfaces through formation of strontium hydroxide journal, November 1998

In situ surface/interface x-ray diffractometer for oxide molecular beam epitaxy journal, January 2016

Surface of Strontium Titanate journal, February 2007

Termination interference along crystal truncation rods of layered crystals journal, November 2004

A Thin Film Approach to Engineering Functionality into Oxides journal, August 2008

Superconducting Interfaces Between Insulating Oxides journal, August 2007

Metallic and Insulating Oxide Interfaces Controlled by Electronic Correlations journal, February 2011

Epitaxial Growth Process of La _0.7 Ca _0.3 MnO ₃ Thin Films on SrTiO ₃ (001): Thickness-Dependent Inhomogeneity Caused by Excess Ti Atoms
journal, March 2014

A Single-Atom-Thick TiO ₂ Nanomesh on an Insulating Oxide
journal, August 2015

Structure of the Photo-catalytically Active Surface of SrTiO ₃
journal, June 2016

Interface-induced superconductivity and strain-dependent spin density waves in FeSe/SrTiO3 thin films
journal, May 2013

Surface Structures of SrTiO ₃ (001): A TiO ₂ -rich Reconstruction with a c(4 × 2) Unit Cell
journal, August 2003

Two-Dimensional Superconducting Phase in ${LaTiO}_{3} / {SrTiO}_{3}$ Heterostructures Induced by High-Mobility Carrier Doping
journal, June 2012

Metallic and Insulating Oxide Interfaces Controlled by Electronic Correlations
journal, February 2011

Two-Dimensional Electron Gases at Complex Oxide Interfaces
journal, July 2014

Superconductivity above 100 K in single-layer FeSe films on doped SrTiO3
journal, November 2014

Filling dependence of electronic properties on the verge of metal–Mott-insulator transition in ${Sr}_{1 - x}$ ${La}_{x}$ ${TiO}_{3}$
journal, April 1993

Atomically precise interfaces from non-stoichiometric deposition
journal, August 2014

Atomic-Scale Visualization of Initial Growth of Homoepitaxial SrTiO ₃ Thin Film on an Atomically Ordered Substrate
journal, September 2011

The structure and chemistry of the TiO2-rich surface of SrTiO3 (001)
journal, September 2002

Realization of atomically flat steps and terraces like surface of SrTiO3 (001) single crystal by hot water etching and high temperature annealing
journal, July 2015

Elastic Constants of Strontium Titanate
journal, January 1963

Quantum many-body interactions in digital oxide superlattices
journal, August 2012

X-Ray Scattering Studies of the Surface Structure of Complex Oxide Films during Layer-by-Layer Growth via Pulsed Laser Deposition
journal, July 2009

Surfactant-mediated molecular beam epitaxy of strained layer semiconductor heterostructures
journal, August 1993

Atomic control and characterization of surface defect states of TiO2 terminated SrTiO3 single crystals
journal, August 2008

Universal Ti-rich termination of atomically flat SrTiO3 (001), (110), and (111) surfaces
journal, January 2011

Vapor deposition processes for amorphous carbon films with sp ³ fractions approaching diamond
journal, August 1991

Atomic Control of the SrTiO₃ Crystal Surface
journal, December 1994

Correlated Oxide Physics and Electronics
journal, July 2014

Nucleation, coarsening, and coalescence during layer-by-layer growth of complex oxides via pulsed laser deposition: Time-resolved, diffuse X-ray scattering studies
journal, November 2010

Two-dimensional superconductivity at a Mott insulator/band insulator interface LaTiO3/SrTiO3
journal, October 2010

Surface transmission electron diffraction for SrTiO3 surfaces
journal, January 2012

High mobility conduction at (110) and (111) LaAlO3/SrTiO3 interfaces
journal, October 2012

A Thin Film Approach to Engineering Functionality into Oxides
journal, August 2008

Surface determination through atomically resolved secondary-electron imaging
journal, June 2015

In situ surface/interface x-ray diffractometer for oxide molecular beam epitaxy
journal, January 2016

Experimental verification of the phonon dispersion curves of strontium titanate
journal, October 1976

Epitaxial growth and electronic structure of LaTiOx films
journal, May 2002

Mechanisms of charge transfer and redistribution in LaAlO3/SrTiO3 revealed by high-energy optical conductivity
journal, April 2014

TiO2-rich reconstructions of SrTiO3(001): a theoretical study of structural patterns
journal, December 2004

Multiband superconductivity and nanoscale inhomogeneity at oxide interfaces
journal, July 2013

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

Ab Initio Predictions of Double-Layer TiO ₂ -Terminated SrTiO ₃ (001) Surface Reconstructions
journal, August 2018

Transport in ferromagnetic GdTiO3/SrTiO3 heterostructures
journal, March 2011

Measurements of Surface Diffusivity and Coarsening during Pulsed Laser Deposition
journal, December 2009

Emergent phenomena at oxide interfaces
journal, January 2012

A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface
journal, January 2004

Tunable Quasi-Two-Dimensional Electron Gases in Oxide Heterostructures
journal, September 2006

Characterization of the X-ray coherence properties of an undulator beamline at the Advanced Photon Source
journal, June 2018

Metallic and Insulating Interfaces of Amorphous SrTiO ₃ -Based Oxide Heterostructures
journal, September 2011

Superconducting Interfaces Between Insulating Oxides
journal, August 2007

The (2×2) reconstructions on the SrTiO3 (001) surface: A combined scanning tunneling microscopy and density functional theory study
journal, September 2011

Direct observation of a two-dimensional hole gas at oxide interfaces
journal, February 2018

Photoemission from Buried Interfaces in ${SrTiO}_{3} / {LaTiO}_{3}$ Superlattices
journal, August 2006

Crystal truncation rods from miscut surfaces
journal, May 2017

Artificial charge-modulationin atomic-scale perovskite titanate superlattices
journal, September 2002

A high-mobility two-dimensional electron gas at the spinel/perovskite interface of γ-Al2O3/SrTiO3
journal, January 2013

Vacant-Site Octahedral Tilings on ${SrTiO}_{3}$ (001), the $(\sqrt{13} \times \sqrt{13}) R 33.7 °$ Surface, and Related Structures
journal, April 2011

Quasi-ideal strontium titanate crystal surfaces through formation of strontium hydroxide
journal, November 1998

Layer-by-Layer Evolution of a Two-Dimensional Electron Gas Near an Oxide Interface
journal, September 2013

Interfacial dielectric layer as an origin of polarization fatigue in ferroelectric capacitors
journal, April 2020

Measurements of Surface Diffusivity and Coarsening During Pulsed Laser Deposition
text, January 2009

Multi-band superconductivity and nanoscale inhomogeneity at oxide interfaces
text, January 2013

Crystal truncation rods from miscut surfaces
text, January 2017

A Single-Atom-Thick TiO ₂ Nanomesh on an Insulating Oxide
journal, August 2015

Epitaxial Growth Process of La _0.7 Ca _0.3 MnO ₃ Thin Films on SrTiO ₃ (001): Thickness-Dependent Inhomogeneity Caused by Excess Ti Atoms
journal, March 2014

Surface Structures of SrTiO ₃ (001): A TiO ₂ -rich Reconstruction with a c(4 × 2) Unit Cell
journal, August 2003

Structure of the Photo-catalytically Active Surface of SrTiO ₃
journal, June 2016

Edge effects
journal, September 2002

Artificial charge-modulationin atomic-scale perovskite titanate superlattices
journal, September 2002

Two-dimensional superconductivity at a Mott insulator/band insulator interface LaTiO3/SrTiO3
journal, October 2010

A high-mobility two-dimensional electron gas at the spinel/perovskite interface of γ-Al2O3/SrTiO3
journal, January 2013

Emergent phenomena at oxide interfaces
journal, January 2012

Superconductivity above 100 K in single-layer FeSe films on doped SrTiO3
journal, November 2014

2D hole gas seen
journal, February 2018

Quasi-ideal strontium titanate crystal surfaces through formation of strontium hydroxide
journal, November 1998

In situ surface/interface x-ray diffractometer for oxide molecular beam epitaxy
journal, January 2016

Surface of Strontium Titanate
journal, February 2007

Termination interference along crystal truncation rods of layered crystals
journal, November 2004

A Thin Film Approach to Engineering Functionality into Oxides
journal, August 2008

Superconducting Interfaces Between Insulating Oxides
journal, August 2007

Metallic and Insulating Oxide Interfaces Controlled by Electronic Correlations
journal, February 2011

Atomic Control of the SrTiO₃ Crystal Surface
journal, December 1994

Measurements of Surface Diffusivity and Coarsening During Pulsed Laser Deposition
text, January 2009

High mobility conduction at (110) and (111) LaAlO3/SrTiO3 interfaces
text, January 2012

Multi-band superconductivity and nanoscale inhomogeneity at oxide interfaces
text, January 2013