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Title: Emergence of the Vortex State in Confined Ferroelectric Heterostructures

Abstract

The manipulation of charge and lattice degrees of freedom in atomically precise, low-dimensional ferroelectric superlattices can lead to exotic polar structures, such as a vortex state. The role of interfaces in the evolution of the vortex state in these superlattices (and the associated electrostatic and elastic boundary conditions they produce) has remained unclear. Here, the toroidal state, arranged in arrays of alternating clockwise/counterclockwise polar vortices, in a confined SrTiO$$_3$$/PbTiO$$_3$$/SrTiO$$_3$$ trilayer is investigated. By utilizing a combination of transmission electron microscopy, synchrotron-based X-ray diffraction, and phase-field modeling, the phase transition as a function of layer thickness (number of unit cells) demonstrates how the vortex state emerges from the ferroelectric state by varying the thickness of the confined PbTiO$$_3$$ layer. Intriguingly, the vortex state arises at head-to-head domain boundaries in ferroelectric α$$_1$$/α$$_2$$ twin structures. In turn, by varying the total number of PbTiO$$_3$$ layers (moving from trilayer to superlattices), it is possible to manipulate the long-range interactions among multiple confined PbTiO$$_3$$ layers to stabilize the vortex state. Finally, this work provides a new understanding of how the different energies work together to produce this exciting new state of matter and can contribute to the design of novel states and potential memory applications.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [3];  [5];  [1];  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States)
  3. Pennsylvania State Univ., University Park, PA (United States)
  4. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Gordon and Betty Moore Foundation (GBMF)
OSTI Identifier:
1633242
Alternate Identifier(s):
OSTI ID: 1543168
Grant/Contract Number:  
AC02-05CH11231; AC02-06CH11357; FG02-07ER46417; DGE-1106400; DMR-1420620; DMR-1210588; GBMF5307; AC02‐06CH11357; FG02‐07ER46417
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 36; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Hsu, Shang‐Lin, McCarter, Margaret R., Dai, Cheng, Hong, Zijian, Chen, Long‐Qing, Nelson, Christopher T., Martin, Lane W., and Ramesh, Ramamoorthy. Emergence of the Vortex State in Confined Ferroelectric Heterostructures. United States: N. p., 2019. Web. https://doi.org/10.1002/adma.201901014.
Hsu, Shang‐Lin, McCarter, Margaret R., Dai, Cheng, Hong, Zijian, Chen, Long‐Qing, Nelson, Christopher T., Martin, Lane W., & Ramesh, Ramamoorthy. Emergence of the Vortex State in Confined Ferroelectric Heterostructures. United States. https://doi.org/10.1002/adma.201901014
Hsu, Shang‐Lin, McCarter, Margaret R., Dai, Cheng, Hong, Zijian, Chen, Long‐Qing, Nelson, Christopher T., Martin, Lane W., and Ramesh, Ramamoorthy. Fri . "Emergence of the Vortex State in Confined Ferroelectric Heterostructures". United States. https://doi.org/10.1002/adma.201901014. https://www.osti.gov/servlets/purl/1633242.
@article{osti_1633242,
title = {Emergence of the Vortex State in Confined Ferroelectric Heterostructures},
author = {Hsu, Shang‐Lin and McCarter, Margaret R. and Dai, Cheng and Hong, Zijian and Chen, Long‐Qing and Nelson, Christopher T. and Martin, Lane W. and Ramesh, Ramamoorthy},
abstractNote = {The manipulation of charge and lattice degrees of freedom in atomically precise, low-dimensional ferroelectric superlattices can lead to exotic polar structures, such as a vortex state. The role of interfaces in the evolution of the vortex state in these superlattices (and the associated electrostatic and elastic boundary conditions they produce) has remained unclear. Here, the toroidal state, arranged in arrays of alternating clockwise/counterclockwise polar vortices, in a confined SrTiO$_3$/PbTiO$_3$/SrTiO$_3$ trilayer is investigated. By utilizing a combination of transmission electron microscopy, synchrotron-based X-ray diffraction, and phase-field modeling, the phase transition as a function of layer thickness (number of unit cells) demonstrates how the vortex state emerges from the ferroelectric state by varying the thickness of the confined PbTiO$_3$ layer. Intriguingly, the vortex state arises at head-to-head domain boundaries in ferroelectric α$_1$/α$_2$ twin structures. In turn, by varying the total number of PbTiO$_3$ layers (moving from trilayer to superlattices), it is possible to manipulate the long-range interactions among multiple confined PbTiO$_3$ layers to stabilize the vortex state. Finally, this work provides a new understanding of how the different energies work together to produce this exciting new state of matter and can contribute to the design of novel states and potential memory applications.},
doi = {10.1002/adma.201901014},
journal = {Advanced Materials},
number = 36,
volume = 31,
place = {United States},
year = {2019},
month = {7}
}

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    Works referencing / citing this record:

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