skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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 LaTiO 3on SrTiO 3(001), we find that a TiO 2adlayer 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 TiO 2adlayer 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 TiO 2-terminated SrTiO 3(001) and demonstrates the critical role of excess TiO 2surface stoichiometry on the initial stages of heteroepitaxial growth on this important perovskite oxide substrate material.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [3];  [4]; ORCiD logo [3]
  1. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); James Madison Univ., Harrisonburg, VA (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
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.
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. doi:10.1126/sciadv.aav0764.
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. doi:10.1126/sciadv.aav0764. https://www.osti.gov/servlets/purl/1524409.
@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 = {2019},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

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

  • Shimizu, Ryota; Ohsawa, Takeo; Iwaya, Katsuya
  • Crystal Growth & Design, Vol. 14, Issue 4
  • DOI: 10.1021/cg4013119

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

  • Plaza, Manuel; Huang, Xin; Ko, J. Y. Peter
  • Journal of the American Chemical Society, Vol. 138, Issue 25
  • DOI: 10.1021/jacs.6b03338

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

  • Tan, Shiyong; Zhang, Yan; Xia, Miao
  • Nature Materials, Vol. 12, Issue 7
  • DOI: 10.1038/nmat3654

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

  • Erdman, Natasha; Warschkow, Oliver; Asta, Mark
  • Journal of the American Chemical Society, Vol. 125, Issue 33
  • DOI: 10.1021/ja034933h

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

  • Ge, Jian-Feng; Liu, Zhi-Long; Liu, Canhua
  • Nature Materials, Vol. 14, Issue 3
  • DOI: 10.1038/nmat4153

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

  • Nie, Y. F.; Zhu, Y.; Lee, C. -H.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5530

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

  • Shimizu, Ryota; Iwaya, Katsuya; Ohsawa, Takeo
  • ACS Nano, Vol. 5, Issue 10
  • DOI: 10.1021/nn202477n

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

  • Erdman, Natasha; Poeppelmeier, Kenneth R.; Asta, Mark
  • Nature, Vol. 419, Issue 6902
  • DOI: 10.1038/nature01010

Elastic Constants of Strontium Titanate
journal, January 1963


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

  • Monkman, Eric J.; Adamo, Carolina; Mundy, Julia A.
  • Nature Materials, Vol. 11, Issue 10
  • DOI: 10.1038/nmat3405

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

  • Brock, J. D.; Ferguson, J. D.; Woll, A. R.
  • Metallurgical and Materials Transactions A, Vol. 41, Issue 5
  • DOI: 10.1007/s11661-009-9910-5

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


Surface of Strontium Titanate
journal, February 2007


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

  • Kareev, M.; Prosandeev, S.; Liu, J.
  • Applied Physics Letters, Vol. 93, Issue 6
  • DOI: 10.1063/1.2971035

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

  • Biswas, A.; Rossen, P. B.; Yang, C. -H.
  • Applied Physics Letters, Vol. 98, Issue 5
  • DOI: 10.1063/1.3549860

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

  • Cuomo, Jerome J.; Pappas, David L.; Bruley, John
  • Journal of Applied Physics, Vol. 70, Issue 3
  • DOI: 10.1063/1.349540

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

  • Brock, J. D.; Ferguson, J. D.; Kim, Yongsam
  • Materials Science and Engineering: A, Vol. 528, Issue 1
  • DOI: 10.1016/j.msea.2010.07.053

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

  • Biscaras, J.; Bergeal, N.; Kushwaha, A.
  • Nature Communications, Vol. 1, Issue 1
  • DOI: 10.1038/ncomms1084

Surface transmission electron diffraction for SrTiO3 surfaces
journal, January 2012

  • Kienzle, Danielle M.; Marks, Laurence D.
  • CrystEngComm, Vol. 14, Issue 23
  • DOI: 10.1039/c2ce25204j

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

  • Herranz, G.; Sánchez, F.; Dix, N.
  • Scientific Reports, Vol. 2, Issue 1
  • DOI: 10.1038/srep00758

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


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

  • Ciston, J.; Brown, H. G.; D’Alfonso, A. J.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8358

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

  • Lee, J. H.; Tung, I. C.; Chang, S. -H.
  • Review of Scientific Instruments, Vol. 87, Issue 1
  • DOI: 10.1063/1.4939100

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


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

  • Ohtomo, A.; Muller, D. A.; Grazul, J. L.
  • Applied Physics Letters, Vol. 80, Issue 21
  • DOI: 10.1063/1.1481767

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

  • Asmara, T. C.; Annadi, A.; Santoso, I.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4663

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


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

  • Cook, Seyoung; Marks, Laurence D.
  • The Journal of Physical Chemistry C, Vol. 122, Issue 38
  • DOI: 10.1021/acs.jpcc.8b07128

Transport in ferromagnetic GdTiO3/SrTiO3 heterostructures
journal, March 2011

  • Moetakef, Pouya; Zhang, Jack Y.; Kozhanov, Alexander
  • Applied Physics Letters, Vol. 98, Issue 11
  • DOI: 10.1063/1.3568894

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


Emergent phenomena at oxide interfaces
journal, January 2012

  • Hwang, H. Y.; Iwasa, Y.; Kawasaki, M.
  • Nature Materials, Vol. 11, Issue 2
  • DOI: 10.1038/nmat3223

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


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

  • Chen, Yunzhong; Pryds, Nini; Kleibeuker, Josée E.
  • Nano Letters, Vol. 11, Issue 9
  • DOI: 10.1021/nl201821j

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

  • Ohtomo, A.; Muller, D. A.; Grazul, J. L.
  • Nature, Vol. 419, Issue 6905
  • DOI: 10.1038/nature00977

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

  • Chen, Y. Z.; Bovet, N.; Trier, F.
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2394

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

  • Koster, Gertjan; Kropman, Boike L.; Rijnders, Guus J. H. M.
  • Applied Physics Letters, Vol. 73, Issue 20
  • DOI: 10.1063/1.122630

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