DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Multiscale electric-field imaging of polarization vortex structures in PbTiO3/SrTiO3 superlattices

Abstract

In ferroelectric heterostructures, the interaction between intrinsic polarization and the electric field generates a rich set of localized electrical properties. The local electric field is determined by several connected factors, including the charge distribution of individual unit cells, the interfacial electromechanical boundary conditions, and chemical composition of the interfaces. However, especially in ferroelectric perovskites, a complete description of the local electric field across micro-, nano-, and atomic-length scales is missing. Here, by applying four-dimensional scanning transmission electron microscopy (4D STEM) with multiple probe sizes matching the size of structural features, we directly image the electric field of polarization vortices in (PbTiO3)16/(SrTiO3)16 superlattices and reveal different electric field configurations corresponding to the atomic scale electronic ordering and the nanoscale boundary conditions. The separability of two different fields probed by 4D STEM offers the possibility to reveal how each contributes to the electronic properties of the film.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. University of California, Irvine, CA (United States)
  2. The Pennsylvania State University, University Park, PA (United States)
  3. University of California, Berkeley, CA (United States)
  4. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF)
OSTI Identifier:
2229303
Grant/Contract Number:  
AC02-05CH11231; SC0014430; SC0020145; ACI-1548562; TG-DMR1700006
Resource Type:
Accepted Manuscript
Journal Name:
APL Materials
Additional Journal Information:
Journal Volume: 11; Journal Issue: 5; Journal ID: ISSN 2166-532X
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Superlattices; Electrical properties and parameters; Electronic devices; Heterostructures; Electric fields; Electron diffraction; Ferroelectric materials; Perovskites, Thin films; Transmission electron microscopy

Citation Formats

Addiego, Christopher, Zorn, Jacob A., Gao, Wenpei, Das, Sujit, Guo, Jiaqi, Qu, Chengqing, Zhao, Liming, Martin, Lane W., Ramesh, Ramamoorthy, Chen, Long-Qing, and Pan, Xiaoqing. Multiscale electric-field imaging of polarization vortex structures in PbTiO3/SrTiO3 superlattices. United States: N. p., 2023. Web. doi:10.1063/5.0146713.
Addiego, Christopher, Zorn, Jacob A., Gao, Wenpei, Das, Sujit, Guo, Jiaqi, Qu, Chengqing, Zhao, Liming, Martin, Lane W., Ramesh, Ramamoorthy, Chen, Long-Qing, & Pan, Xiaoqing. Multiscale electric-field imaging of polarization vortex structures in PbTiO3/SrTiO3 superlattices. United States. https://doi.org/10.1063/5.0146713
Addiego, Christopher, Zorn, Jacob A., Gao, Wenpei, Das, Sujit, Guo, Jiaqi, Qu, Chengqing, Zhao, Liming, Martin, Lane W., Ramesh, Ramamoorthy, Chen, Long-Qing, and Pan, Xiaoqing. Thu . "Multiscale electric-field imaging of polarization vortex structures in PbTiO3/SrTiO3 superlattices". United States. https://doi.org/10.1063/5.0146713. https://www.osti.gov/servlets/purl/2229303.
@article{osti_2229303,
title = {Multiscale electric-field imaging of polarization vortex structures in PbTiO3/SrTiO3 superlattices},
author = {Addiego, Christopher and Zorn, Jacob A. and Gao, Wenpei and Das, Sujit and Guo, Jiaqi and Qu, Chengqing and Zhao, Liming and Martin, Lane W. and Ramesh, Ramamoorthy and Chen, Long-Qing and Pan, Xiaoqing},
abstractNote = {In ferroelectric heterostructures, the interaction between intrinsic polarization and the electric field generates a rich set of localized electrical properties. The local electric field is determined by several connected factors, including the charge distribution of individual unit cells, the interfacial electromechanical boundary conditions, and chemical composition of the interfaces. However, especially in ferroelectric perovskites, a complete description of the local electric field across micro-, nano-, and atomic-length scales is missing. Here, by applying four-dimensional scanning transmission electron microscopy (4D STEM) with multiple probe sizes matching the size of structural features, we directly image the electric field of polarization vortices in (PbTiO3)16/(SrTiO3)16 superlattices and reveal different electric field configurations corresponding to the atomic scale electronic ordering and the nanoscale boundary conditions. The separability of two different fields probed by 4D STEM offers the possibility to reveal how each contributes to the electronic properties of the film.},
doi = {10.1063/5.0146713},
journal = {APL Materials},
number = 5,
volume = 11,
place = {United States},
year = {Thu May 04 00:00:00 EDT 2023},
month = {Thu May 04 00:00:00 EDT 2023}
}

Works referenced in this record:

Creating emergent phenomena in oxide superlattices
journal, March 2019


First-principles studies of lone-pair-induced distortions in epitaxial phases of perovskite SnTiO 3 and PbTiO 3
journal, January 2015


Atomic-scale quantification of charge densities in two-dimensional materials
journal, September 2018


Theoretical investigation of magnetoelectric behavior in Bi Fe O 3
journal, December 2006


Towards the Development of Flexible Non-Volatile Memories
journal, August 2013


Spatially resolved steady-state negative capacitance
journal, January 2019


Direct Visualization of Local Electromagnetic Field Structures by Scanning Transmission Electron Microscopy
journal, July 2017


Intrinsic Conductance of Domain Walls in BiFeO 3
journal, June 2019


Structures and electronic properties of domain walls in BiFeO3 thin films
journal, July 2019

  • Huyan, Huaixun; Li, Linze; Addiego, Christopher
  • National Science Review, Vol. 6, Issue 4
  • DOI: 10.1093/nsr/nwz101

Influence of lens aberrations, specimen thickness and tilt on differential phase contrast STEM images
journal, December 2020


Real-space charge-density imaging with sub-ångström resolution by four-dimensional electron microscopy
journal, October 2019


Probing the Internal Atomic Charge Density Distributions in Real Space
journal, August 2018

  • Sánchez-Santolino, Gabriel; Lugg, Nathan R.; Seki, Takehito
  • ACS Nano, Vol. 12, Issue 9
  • DOI: 10.1021/acsnano.8b03712

Imaging individual atoms inside crystals with ADF-STEM
journal, September 2003


Direct Measurement of Polarization-Induced Fields in GaN/AlN by Nano-Beam Electron Diffraction
journal, June 2016

  • Carvalho, Daniel; Müller-Caspary, Knut; Schowalter, Marco
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep28459

Electrical Polarization in AlN/GaN Nanodisks Measured by Momentum-Resolved 4D Scanning Transmission Electron Microscopy
journal, March 2019


Emerging memories: resistive switching mechanisms and current status
journal, June 2012


Anisotropic polarization-induced conductance at a ferroelectric–insulator interface
journal, September 2018


Discovery of a magnetic conductive interface in PbZr0.2Ti0.8O3 /SrTiO3 heterostructures
journal, February 2018


Two-dimensional electron gas at the Ti-diffused BiFeO 3 /SrTiO 3 interface
journal, July 2015

  • Chen, Chunlin; Lv, Shuhui; Li, Junjie
  • Applied Physics Letters, Vol. 107, Issue 3
  • DOI: 10.1063/1.4926732

Strain mapping at nanometer resolution using advanced nano-beam electron diffraction
journal, June 2015

  • Ozdol, V. B.; Gammer, C.; Jin, X. G.
  • Applied Physics Letters, Vol. 106, Issue 25
  • DOI: 10.1063/1.4922994

Direct electric field imaging of graphene defects
journal, September 2018


Thickness and defocus dependence of inter-atomic electric fields measured by scanning diffraction
journal, January 2020


XSEDE: Accelerating Scientific Discovery
journal, September 2014

  • Towns, John; Cockerill, Timothy; Dahan, Maytal
  • Computing in Science & Engineering, Vol. 16, Issue 5
  • DOI: 10.1109/MCSE.2014.80

Origin of ferroelectricity in perovskite oxides
journal, July 1992


Electric field imaging of single atoms
journal, May 2017

  • Shibata, Naoya; Seki, Takehito; Sánchez-Santolino, Gabriel
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15631

Giant Resistive Switching via Control of Ferroelectric Charged Domain Walls
journal, May 2016

  • Li, Linze; Britson, Jason; Jokisaari, Jacob R.
  • Advanced Materials, Vol. 28, Issue 31
  • DOI: 10.1002/adma.201600160

Differential phase-contrast microscopy at atomic resolution
journal, June 2012

  • Shibata, Naoya; Findlay, Scott D.; Kohno, Yuji
  • Nature Physics, Vol. 8, Issue 8
  • DOI: 10.1038/nphys2337

Controllable conductive readout in self-assembled, topologically confined ferroelectric domain walls
journal, July 2018


Periodic Giant Polarization Gradients in Doped BiFeO 3 Thin Films
journal, January 2018


Mapping 1D Confined Electromagnetic Edge States in 2D Monolayer Semiconducting MoS2 Using 4D-STEM
journal, March 2022


Direct visualization of anionic electrons in an electride reveals inhomogeneities
journal, April 2021

  • Zheng, Qiang; Feng, Tianli; Hachtel, Jordan A.
  • Science Advances, Vol. 7, Issue 15
  • DOI: 10.1126/sciadv.abe6819

Atomic electrostatic maps of 1D channels in 2D semiconductors using 4D scanning transmission electron microscopy
journal, March 2019


Local negative permittivity and topological phase transition in polar skyrmions
journal, October 2020


Atomic electric fields revealed by a quantum mechanical approach to electron picodiffraction
journal, December 2014

  • Müller, Knut; Krause, Florian F.; Béché, Armand
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6653

Strain Tuning of Ferroelectric Thin Films
journal, August 2007


Device Physics of Ferroelectric Thin-Film Memories
journal, April 1999

  • Scott, J. F.
  • Japanese Journal of Applied Physics, Vol. 38, Issue Part 1, No. 4B
  • DOI: 10.1143/jjap.38.2272