Relating electronic and geometric structure of atomic layer deposited BaTiO3 to its electrical properties

Torgersen, Jan; Acharya, Shinjita; Dadlani, Anup Lal; Petousis, Ioannis; Kim, Yongmin; Trejo, Orlando; Nordlund, Dennis; Prinz, Fritz B.

doi:10.1021/acs.jpclett.6b00393

Title: Relating electronic and geometric structure of atomic layer deposited BaTiO₃ to its electrical properties

Abstract

Atomic layer deposition allows the fabrication of BaTiO₃ (BTO) ultrathin films with tunable dielectric properties, which is a promising material for electronic and optical technology. Industrial applicability necessitates a better understanding of their atomic structure and corresponding properties. Through the use of element-specific X-ray absorption near edge structure (XANES) analysis, O K-edge of BTO as a function of cation composition and underlying substrate (RuO₂ and SiO₂) is revealed. By employing density functional theory and multiple scattering simulations, we analyze the distortions in BTO’s bonding environment captured by the XANES spectra. The spectral weight shifts to lower energy with increasing Ti content and provides an atomic scale (microscopic) explanation for the increase in leakage current density. Differences in film morphologies in the first few layers near substrate–film interfaces reveal BTO’s homogeneous growth on RuO₂ and its distorted growth on SiO₂. As a result, this work links structural changes to BTO thin-film properties and provides insight necessary for optimizing future BTO and other ternary metal oxide-based thin-film devices.

Authors:

Torgersen, Jan ^[1]; Acharya, Shinjita ^[1]; Dadlani, Anup Lal ^[1]; Petousis, Ioannis ^[1]; Kim, Yongmin ^[1]; Trejo, Orlando ^[1]; Nordlund, Dennis ^[2]; Prinz, Fritz B. ^[1]

Stanford Univ., Stanford, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

Publication Date:: Thu Mar 24 00:00:00 EDT 2016

Research Org.:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

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

OSTI Identifier:: 1249098

Grant/Contract Number:: J3505-N20

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry Letters

Additional Journal Information:: Journal Volume: 7; Journal Issue: 8; Journal ID: ISSN 1948-7185

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats


                    Torgersen, Jan, Acharya, Shinjita, Dadlani, Anup Lal, Petousis, Ioannis, Kim, Yongmin, Trejo, Orlando, Nordlund, Dennis, and Prinz, Fritz B. Relating electronic and geometric structure of atomic layer deposited BaTiO3 to its electrical properties.  United States: N. p., 2016. 
Web.  doi:10.1021/acs.jpclett.6b00393.

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                    Torgersen, Jan, Acharya, Shinjita, Dadlani, Anup Lal, Petousis, Ioannis, Kim, Yongmin, Trejo, Orlando, Nordlund, Dennis, & Prinz, Fritz B. Relating electronic and geometric structure of atomic layer deposited BaTiO3 to its electrical properties.  United States.  https://doi.org/10.1021/acs.jpclett.6b00393

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                    Torgersen, Jan, Acharya, Shinjita, Dadlani, Anup Lal, Petousis, Ioannis, Kim, Yongmin, Trejo, Orlando, Nordlund, Dennis, and Prinz, Fritz B. Thu .  
"Relating electronic and geometric structure of atomic layer deposited BaTiO3 to its electrical properties".  United States.  https://doi.org/10.1021/acs.jpclett.6b00393.  https://www.osti.gov/servlets/purl/1249098.

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@article{osti_1249098,

  title        = {Relating electronic and geometric structure of atomic layer deposited BaTiO3 to its electrical properties},

  author       = {Torgersen, Jan and Acharya, Shinjita and Dadlani, Anup Lal and Petousis, Ioannis and Kim, Yongmin and Trejo, Orlando and Nordlund, Dennis and Prinz, Fritz B.},

  abstractNote = {Atomic layer deposition allows the fabrication of BaTiO3 (BTO) ultrathin films with tunable dielectric properties, which is a promising material for electronic and optical technology. Industrial applicability necessitates a better understanding of their atomic structure and corresponding properties. Through the use of element-specific X-ray absorption near edge structure (XANES) analysis, O K-edge of BTO as a function of cation composition and underlying substrate (RuO2 and SiO2) is revealed. By employing density functional theory and multiple scattering simulations, we analyze the distortions in BTO’s bonding environment captured by the XANES spectra. The spectral weight shifts to lower energy with increasing Ti content and provides an atomic scale (microscopic) explanation for the increase in leakage current density. Differences in film morphologies in the first few layers near substrate–film interfaces reveal BTO’s homogeneous growth on RuO2 and its distorted growth on SiO2. As a result, this work links structural changes to BTO thin-film properties and provides insight necessary for optimizing future BTO and other ternary metal oxide-based thin-film devices.},

  doi          = {10.1021/acs.jpclett.6b00393},

  journal      = {Journal of Physical Chemistry Letters},

  number       = 8,

  volume       = 7,

  place        = {United States},

  year         = {Thu Mar 24 00:00:00 EDT 2016},

  month        = {Thu Mar 24 00:00:00 EDT 2016}

}

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https://doi.org/10.1021/acs.jpclett.6b00393

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Works referencing / citing this record:

Atomic layer deposition of perovskites part 2: Designing next generation electronic applications
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Bin Afif, Abdulla; Dadlani, Anup L.; Burgmann, Stephanie
Material Design & Processing Communications, Vol. 2, Issue 1
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Title: Relating electronic and geometric structure of atomic layer deposited BaTiO3 to its electrical properties

Abstract

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Structural and electrical properties of rf‐sputtered amorphous barium titanate thin films journal, December 1987

Synthesis of Single-Crystalline Perovskite Nanorods Composed of Barium Titanate and Strontium Titanate journal, February 2002

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Full-PAW calculations of XANES/ELNES spectra of Ti-bearing oxide crystals and TiO-SiO glasses: Relation between pre-edge peaks and Ti coordination journal, May 2012

Growth of Conductive SrRuO 3 Films by Combining Atomic Layer Deposited SrO and Chemical Vapor Deposited RuO 2 Layers journal, December 2012

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Interfaces and Composition Profiles in Metal–Sulfide Nanolayers Synthesized by Atomic Layer Deposition
journal, January 2013

Crystallinity of inorganic films grown by atomic layer deposition: Overview and general trends
journal, January 2013

Plasma Processing for Crystallization and Densification of Atomic Layer Deposition BaTiO ₃ Thin Films
journal, June 2014

Effects of crystallization on the electrical properties of ultrathin HfO2 dielectrics grown by atomic layer deposition
journal, January 2003

High charge storage in amorphous BaTiO ₃ thin films
journal, June 1991

Diffuse Phase Transition in Epitaxial BaTiO3 Thin Films
journal, March 2002

Ferroelectric properties of SrRuO3∕BaTiO3∕SrRuO3 ultrathin film capacitors free from passive layers
journal, February 2006

Exploring the local electronic structure and geometric arrangement of ALD Zn(O,S) buffer layers using X-ray absorption spectroscopy
journal, January 2015

Quantifying Geometric Strain at the PbS QD-TiO ₂ Anode Interface and Its Effect on Electronic Structures
journal, November 2015

EXAFS studies of MeO3−x (Me = W, Mo, Re, Ir) crystalline and amorphous oxides
journal, October 1991

Evolution of Crystal Structure During the Initial Stages of ZnO Atomic Layer Deposition
journal, January 2016

The Problem with Determining Atomic Structure at the Nanoscale
journal, April 2007

Ab initio theory and calculations of X-ray spectra
journal, July 2009

Parameter-free calculations of X-ray spectra with FEFF9
journal, January 2010

Oxygen 1 $s$ excitation and tetragonal distortion from core-hole effect in BaTiO $_{3}$
journal, November 2013

Oxygen 1 s ELNES study of perovskites (Ca,Sr,Ba)TiO ₃
journal, March 2001

High-resolution x-ray absorption spectroscopy of BaTiO $_{3}$ : Experiment and first-principles calculations
journal, November 2011

Enhancement of Ferroelectricity in Strained BaTiO₃ Thin Films
journal, November 2004

Interface Between Atomic Layer Deposition Ta ₂ O ₅ Films and GaAs(100) Surfaces
journal, April 2012

Comparison of electronic structures of RuO2 and IrO2 nanorods investigated by x-ray absorption and scanning photoelectron microscopy
journal, January 2007

Immobilization of RuO ₂ on Carbon Nanotube: An X-ray Absorption Near-Edge Structure Study
journal, May 2009

Full-PAW calculations of XANES/ELNES spectra of Ti-bearing oxide crystals and TiO-SiO glasses: Relation between pre-edge peaks and Ti coordination
journal, May 2012

Growth of Conductive SrRuO ₃ Films by Combining Atomic Layer Deposited SrO and Chemical Vapor Deposited RuO ₂ Layers
journal, December 2012

Mechanical properties of thin films
journal, November 1989

Studying the effects of Zr-doping in (Bi _0.5 Na _0.5 )TiO ₃ via diffraction and spectroscopy
journal, January 2014

Thickness dependence of room temperature permittivity of polycrystalline BaTiO3 thin films by radio-frequency magnetron sputtering
journal, May 1997

Interface Engineered BaTiO ₃ /SrTiO ₃ Heterostructures with Optimized High-Frequency Dielectric Properties
journal, October 2012

Thickness and temperature dependence of the leakage current in hafnium-based Si SOI MOSFETs
journal, December 2012

Comparison of Nanomechanical Behavior of the Amorphous and Crystalline Phases of ALD HfO2
journal, August 2009

Investigations of the electronic structure of d0 transition metal oxides belonging to the perovskite family
journal, October 2003

Atomic layer deposition of perovskites part 2: Designing next generation electronic applications
journal, December 2019