Effect of buffer termination on intermixing and conductivity in LaTiO3/SrTiO3 heterostructures integrated on Si(100)

Chen, Tongjie; Ahmadi-Majlan, Kamyar; Lim, Zheng Hui; Zhang, Zhan; Ngai, Joseph H.; Kumah, Divine P.

doi:10.1116/6.0001464

Title: Effect of buffer termination on intermixing and conductivity in LaTiO₃/SrTiO₃ heterostructures integrated on Si(100)

Abstract

Here, the control of chemical exchange across heterointerfaces formed between ultrathin functional transition-metal oxide layers provides an effective route to manipulate the electronic properties of these systems. By determining the layer-resolved structural profile across the interface between the Mott insulator, LaTiO₃ (LTO) grown epitaxially on SrTiO₃ (STO)-buffered silicon by molecular beam epitaxy, we find that interfacial cationic exchange depends on the surface termination of the strained STO buffer. Using a combination of temperature-dependent transport and synchrotron x-ray crystal truncation rods and reciprocal space mapping, an enhanced conductivity in STO/LTO/SrO-terminated STO buffers compared to heterostructures with TiO₂-terminated STO buffers is correlated with La/Sr exchange and the formation of metallic La_1-xSr_xTiO₃. La/Sr exchange effectively reduces the strain energy of the system due to the large lattice mismatch between the nominal oxide layers and the Si substrate.

Authors:

Chen, Tongjie ^[1]; Ahmadi-Majlan, Kamyar ^[2]; Lim, Zheng Hui ^[2]; Zhang, Zhan ^[3]; Ngai, Joseph H. ^[2];

^[1]

North Carolina State Univ., Raleigh, NC (United States)
Univ. of Texas-Arlington, TX (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

Publication Date:: Thu Dec 02 00:00:00 EST 2021

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

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

OSTI Identifier:: 1846807

Alternate Identifier(s):: OSTI ID: 1833765

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Vacuum Science and Technology A

Additional Journal Information:: Journal Volume: 40; Journal Issue: 1; Journal ID: ISSN 0734-2101

Publisher:: American Vacuum Society / AIP

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Heterointerfaces; Insulators; Bragg peak; Heterostructures; Electric measurements; Crystal lattices; Epitaxy; X-ray crystal truncation rod scattering; Perovskites; Synchrotrons

Citation Formats


                    Chen, Tongjie, Ahmadi-Majlan, Kamyar, Lim, Zheng Hui, Zhang, Zhan, Ngai, Joseph H., and Kumah, Divine P. Effect of buffer termination on intermixing and conductivity in LaTiO3/SrTiO3 heterostructures integrated on Si(100).  United States: N. p., 2021. 
Web.  doi:10.1116/6.0001464.

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                    Chen, Tongjie, Ahmadi-Majlan, Kamyar, Lim, Zheng Hui, Zhang, Zhan, Ngai, Joseph H., & Kumah, Divine P. Effect of buffer termination on intermixing and conductivity in LaTiO3/SrTiO3 heterostructures integrated on Si(100).  United States.  https://doi.org/10.1116/6.0001464

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                    Chen, Tongjie, Ahmadi-Majlan, Kamyar, Lim, Zheng Hui, Zhang, Zhan, Ngai, Joseph H., and Kumah, Divine P. Thu .  
"Effect of buffer termination on intermixing and conductivity in LaTiO3/SrTiO3 heterostructures integrated on Si(100)".  United States.  https://doi.org/10.1116/6.0001464.  https://www.osti.gov/servlets/purl/1846807.

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@article{osti_1846807,

  title        = {Effect of buffer termination on intermixing and conductivity in LaTiO3/SrTiO3 heterostructures integrated on Si(100)},

  author       = {Chen, Tongjie and Ahmadi-Majlan, Kamyar and Lim, Zheng Hui and Zhang, Zhan and Ngai, Joseph H. and Kumah, Divine P.},

  abstractNote = {Here, the control of chemical exchange across heterointerfaces formed between ultrathin functional transition-metal oxide layers provides an effective route to manipulate the electronic properties of these systems. By determining the layer-resolved structural profile across the interface between the Mott insulator, LaTiO3 (LTO) grown epitaxially on SrTiO3 (STO)-buffered silicon by molecular beam epitaxy, we find that interfacial cationic exchange depends on the surface termination of the strained STO buffer. Using a combination of temperature-dependent transport and synchrotron x-ray crystal truncation rods and reciprocal space mapping, an enhanced conductivity in STO/LTO/SrO-terminated STO buffers compared to heterostructures with TiO2-terminated STO buffers is correlated with La/Sr exchange and the formation of metallic La1-xSrxTiO3. La/Sr exchange effectively reduces the strain energy of the system due to the large lattice mismatch between the nominal oxide layers and the Si substrate.},

  doi          = {10.1116/6.0001464},

  journal      = {Journal of Vacuum Science and Technology A},

  number       = 1,

  volume       = 40,

  place        = {United States},

  year         = {Thu Dec 02 00:00:00 EST 2021},

  month        = {Thu Dec 02 00:00:00 EST 2021}

}

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Title: Effect of buffer termination on intermixing and conductivity in LaTiO3/SrTiO3 heterostructures integrated on Si(100)

Abstract

Citation Formats

Interface-induced phenomena in magnetism journal, June 2017

Whither the oxide interface journal, January 2012

Correlated Oxide Physics and Electronics journal, July 2014

Avoiding the Polarization Catastrophe in LaAlO 3 Overlayers on SrTiO 3 ( 001 ) through Polar Distortion journal, March 2009

Oxygen octahedron reconstruction in the SrTiO 3 / LaAlO 3 heterointerfaces investigated using aberration-corrected ultrahigh-resolution transmission electron microscopy journal, February 2009

Interface Physics in Complex Oxide Heterostructures journal, March 2011

Control of octahedral connectivity in perovskite oxide heterostructures: An emerging route to multifunctional materials discovery journal, March 2012

Why some interfaces cannot be sharp journal, January 2006

The Impacts of Cation Stoichiometry and Substrate Surface Quality on Nucleation, Structure, Defect Formation, and Intermixing in Complex Oxide Heteroepitaxy-LaCrO 3 on SrTiO 3 (001) journal, January 2013

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

Three-dimensional character of the Fermi surface in ultrathin LaTiO 3 / SrTiO 3 heterostructures journal, March 2019

Structural Basis for the Conducting Interface between LaAlO3 and SrTiO3 journal, October 2007

Thermodynamic instability at the stoichiometric LaAlO 3 / SrTiO 3 (001) interface journal, July 2010

Hidden lattice instabilities as origin of the conductive interface between insulating LaAlO3 and SrTiO3 journal, September 2016

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Metallicity in LaTiO 3 thin films induced by lattice deformation journal, April 2010

Origin of metallicity of La Ti O 3 ∕ Sr Ti O 3 heterostructures journal, March 2008

Electronic transition in La 1 − x Sr x TiO 3 journal, October 1999

Optical Study of the Free-Carrier Response of LaTiO 3 / SrTiO 3 Superlattices journal, December 2007

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

A high density two-dimensional electron gas in an oxide heterostructure on Si (001) journal, November 2014

Crystalline Oxides on Silicon: The First Five Monolayers journal, October 1998

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Title: Effect of buffer termination on intermixing and conductivity in LaTiO₃/SrTiO₃ heterostructures integrated on Si(100)

Interface-induced phenomena in magnetism
journal, June 2017

Whither the oxide interface
journal, January 2012

Correlated Oxide Physics and Electronics
journal, July 2014

Avoiding the Polarization Catastrophe in ${LaAlO}_{3}$ Overlayers on ${SrTiO}_{3} (001)$ through Polar Distortion
journal, March 2009

Oxygen octahedron reconstruction in the ${SrTiO}_{3} / {LaAlO}_{3}$ heterointerfaces investigated using aberration-corrected ultrahigh-resolution transmission electron microscopy
journal, February 2009

Interface Physics in Complex Oxide Heterostructures
journal, March 2011

Control of octahedral connectivity in perovskite oxide heterostructures: An emerging route to multifunctional materials discovery
journal, March 2012

Why some interfaces cannot be sharp
journal, January 2006

The Impacts of Cation Stoichiometry and Substrate Surface Quality on Nucleation, Structure, Defect Formation, and Intermixing in Complex Oxide Heteroepitaxy-LaCrO ₃ on SrTiO ₃ (001)
journal, January 2013

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

Three-dimensional character of the Fermi surface in ultrathin ${LaTiO}_{3} / {SrTiO}_{3}$ heterostructures
journal, March 2019

Structural Basis for the Conducting Interface between ${LaAlO}_{3}$ and ${SrTiO}_{3}$
journal, October 2007

Thermodynamic instability at the stoichiometric LaAlO ₃ / SrTiO ₃ (001) interface
journal, July 2010

Hidden lattice instabilities as origin of the conductive interface between insulating LaAlO3 and SrTiO3
journal, September 2016

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

Understanding the mechanism of conductivity at the LaAlO3/SrTiO3(001) interface
journal, July 2011

Electronic phenomena at complex oxide interfaces: insights from first principles
journal, January 2010

Probing the Origin of Interfacial Carriers in SrTiO ₃ –LaCrO ₃ Superlattices
journal, January 2017

Epitaxial Oxides on Semiconductors: From Fundamentals to New Devices
journal, July 2019

The interface of epitaxial SrTiO3 on silicon: in situ and ex situ studies
journal, January 2003

Anomalous lattice expansion of coherently strained ${SrTiO}_{3}$ thin films grown on $Si (001)$ by kinetically controlled sequential deposition
journal, January 2006

Atomic structure of the interface between SrTiO3 thin films and Si(001) substrates
journal, September 2008

Band offset and structure of SrTiO3 /Si(001) heterojunctions
journal, May 2001

Oxide 2D electron gases as a route for high carrier densities on (001) Si
journal, May 2015

Misfit strain driven cation inter-diffusion across an epitaxial multiferroic thin film interface
journal, February 2014

Strain-induced material intermixing of InAs quantum dots in GaAs
journal, January 2000

Crystal and magnetic structure of ${LaTiO}_{3} :$ Evidence for nondegenerate $t_{2 g}$ orbitals
journal, August 2003

Mott insulator to metal transition driven by oxygen incorporation in epitaxial LaTiO ₃ films
journal, December 2019

Metal-insulator transitions in epitaxial LaVO $_{3}$ and LaTiO $_{3}$ films
journal, August 2012

Metallicity in ${LaTiO}_{3}$ thin films induced by lattice deformation
journal, April 2010

Origin of metallicity of $La Ti O_{3} ∕ Sr Ti O_{3}$ heterostructures
journal, March 2008

Electronic transition in ${La}_{1 - x} {Sr}_{x} {TiO}_{3}$
journal, October 1999

Optical Study of the Free-Carrier Response of ${LaTiO}_{3} / {SrTiO}_{3}$ Superlattices
journal, December 2007

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

A high density two-dimensional electron gas in an oxide heterostructure on Si (001)
journal, November 2014

Crystalline Oxides on Silicon: The First Five Monolayers
journal, October 1998

Crystalline Oxides on Silicon
journal, April 2010

The atomic structure and polarization of strained SrTiO3/Si
journal, December 2010

A Ferroelectric Oxide Made Directly on Silicon
journal, April 2009

Interfacial structure of SrZr _x Ti ₁₋ _x O ₃ films on Ge
journal, November 2018

Crystal truncation rods and surface roughness
journal, March 1986

Tuning metal-insulator behavior in LaTiO ₃ /SrTiO ₃ heterostructures integrated directly on Si(100) through control of atomic layer thickness
journal, May 2018

GenX : an extensible X-ray reflectivity refinement program utilizing differential evolution
journal, November 2007

Interfacial structure in epitaxial perovskite oxides on (001) Ge crystal
journal, January 2015