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:
-
- University of California, Irvine, CA (United States)
- The Pennsylvania State University, University Park, PA (United States)
- University of California, Berkeley, CA (United States)
- 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
- Ramesh, Ramamoorthy; Schlom, Darrell G.
- Nature Reviews Materials
First-principles studies of lone-pair-induced distortions in epitaxial phases of perovskite and
journal, January 2015
- Pitike, Krishna Chaitanya; Parker, William D.; Louis, Lydie
- Physical Review B, Vol. 91, Issue 3
Atomic-scale quantification of charge densities in two-dimensional materials
journal, September 2018
- Müller-Caspary, Knut; Duchamp, Martial; Rösner, Malte
- Physical Review B, Vol. 98, Issue 12
Theoretical investigation of magnetoelectric behavior in
journal, December 2006
- Ravindran, P.; Vidya, R.; Kjekshus, A.
- Physical Review B, Vol. 74, Issue 22
Towards the Development of Flexible Non-Volatile Memories
journal, August 2013
- Han, Su-Ting; Zhou, Ye; Roy, V. A. L.
- Advanced Materials, Vol. 25, Issue 38
Manipulating topological transformations of polar structures through real-time observation of the dynamic polarization evolution
journal, October 2019
- Du, K.; Zhang, M.; Dai, C.
- Nature Communications, Vol. 10, Issue 1
Spatially resolved steady-state negative capacitance
journal, January 2019
- Yadav, Ajay K.; Nguyen, Kayla X.; Hong, Zijian
- Nature, Vol. 565, Issue 7740
Direct Visualization of Local Electromagnetic Field Structures by Scanning Transmission Electron Microscopy
journal, July 2017
- Shibata, Naoya; Findlay, Scott D.; Matsumoto, Takao
- Accounts of Chemical Research, Vol. 50, Issue 7
Intrinsic Conductance of Domain Walls in BiFeO 3
journal, June 2019
- Zhang, Yi; Lu, Haidong; Yan, Xingxu
- Advanced Materials, Vol. 31, Issue 36
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
Influence of lens aberrations, specimen thickness and tilt on differential phase contrast STEM images
journal, December 2020
- Bürger, Julius; Riedl, Thomas; Lindner, Jörg K. N.
- Ultramicroscopy, Vol. 219
Real-space charge-density imaging with sub-ångström resolution by four-dimensional electron microscopy
journal, October 2019
- Gao, Wenpei; Addiego, Christopher; Wang, Hui
- Nature, Vol. 575, Issue 7783
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
Imaging individual atoms inside crystals with ADF-STEM
journal, September 2003
- Voyles, P. M.; Grazul, J. L.; Muller, D. A.
- Ultramicroscopy, Vol. 96, Issue 3-4
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
Electrical Polarization in AlN/GaN Nanodisks Measured by Momentum-Resolved 4D Scanning Transmission Electron Microscopy
journal, March 2019
- Müller-Caspary, Knut; Grieb, Tim; Müßener, Jan
- Physical Review Letters, Vol. 122, Issue 10
Emerging memories: resistive switching mechanisms and current status
journal, June 2012
- Jeong, Doo Seok; Thomas, Reji; Katiyar, R. S.
- Reports on Progress in Physics, Vol. 75, Issue 7
Anisotropic polarization-induced conductance at a ferroelectric–insulator interface
journal, September 2018
- Zhang, Yi; Lu, Haidong; Xie, Lin
- Nature Nanotechnology, Vol. 13, Issue 12
Discovery of a magnetic conductive interface in PbZr0.2Ti0.8O3 /SrTiO3 heterostructures
journal, February 2018
- Zhang, Yi; Xie, Lin; Kim, Jeongwoo
- Nature Communications, Vol. 9, Issue 1
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
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
Direct electric field imaging of graphene defects
journal, September 2018
- Ishikawa, Ryo; Findlay, Scott D.; Seki, Takehito
- Nature Communications, Vol. 9, Issue 1
Thickness and defocus dependence of inter-atomic electric fields measured by scanning diffraction
journal, January 2020
- Addiego, Christopher; Gao, Wenpei; Pan, Xiaoqing
- Ultramicroscopy, Vol. 208
XSEDE: Accelerating Scientific Discovery
journal, September 2014
- Towns, John; Cockerill, Timothy; Dahan, Maytal
- Computing in Science & Engineering, Vol. 16, Issue 5
Origin of ferroelectricity in perovskite oxides
journal, July 1992
- Cohen, Ronald E.
- Nature, Vol. 358, Issue 6382
Electric field imaging of single atoms
journal, May 2017
- Shibata, Naoya; Seki, Takehito; Sánchez-Santolino, Gabriel
- Nature Communications, Vol. 8, Issue 1
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
Differential phase-contrast microscopy at atomic resolution
journal, June 2012
- Shibata, Naoya; Findlay, Scott D.; Kohno, Yuji
- Nature Physics, Vol. 8, Issue 8
Dynamical diffraction of high-energy electrons investigated by focal series momentum-resolved scanning transmission electron microscopy at atomic resolution
journal, March 2022
- Robert, H. L.; Lobato, I.; Lyu, F. J.
- Ultramicroscopy, Vol. 233
Controllable conductive readout in self-assembled, topologically confined ferroelectric domain walls
journal, July 2018
- Ma, Ji; Ma, Jing; Zhang, Qinghua
- Nature Nanotechnology, Vol. 13, Issue 10
Periodic Giant Polarization Gradients in Doped BiFeO 3 Thin Films
journal, January 2018
- Campanini, Marco; Erni, Rolf; Yang, Chan−Ho
- Nano Letters, Vol. 18, Issue 2
Mapping 1D Confined Electromagnetic Edge States in 2D Monolayer Semiconducting MoS2 Using 4D-STEM
journal, March 2022
- Wen, Yi; Fang, Shiang; Coupin, Matthew
- ACS Nano, Vol. 16, Issue 4
Four-Dimensional Scanning Transmission Electron Microscopy (4D-STEM): From Scanning Nanodiffraction to Ptychography and Beyond
journal, May 2019
- Ophus, Colin
- Microscopy and Microanalysis, Vol. 25, Issue 3
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
Two-dimensional mapping of polarizations of rhombohedral nanostructures in the tetragonal phase of BaTiO 3 by the combined use of the scanning transmission electron microscopy and convergent-beam electron diffraction methods
journal, August 2013
- Tsuda, Kenji; Yasuhara, Akira; Tanaka, Michiyoshi
- Applied Physics Letters, Vol. 103, Issue 8
Atomic electrostatic maps of 1D channels in 2D semiconductors using 4D scanning transmission electron microscopy
journal, March 2019
- Fang, Shiang; Wen, Yi; Allen, Christopher S.
- Nature Communications, Vol. 10, Issue 1
Local negative permittivity and topological phase transition in polar skyrmions
journal, October 2020
- Das, S.; Hong, Z.; Stoica, V. A.
- Nature Materials, Vol. 20, Issue 2
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
Measurement of atomic electric fields and charge densities from average momentum transfers using scanning transmission electron microscopy
journal, July 2017
- Müller-Caspary, Knut; Krause, Florian F.; Grieb, Tim
- Ultramicroscopy, Vol. 178
Strain Tuning of Ferroelectric Thin Films
journal, August 2007
- Schlom, Darrell G.; Chen, Long-Qing; Eom, Chang-Beom
- Annual Review of Materials Research, Vol. 37, Issue 1
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