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Depth-Resolved X-Ray Photoelectron Spectroscopy Evidence of Intrinsic Polar States in HfO2-Based Ferroelectrics

Hill, Megan O. LU ; Kim, Ji Soo ; Müller, Moritz L. ; Phuyal, Dibya ; Taper, Sunil ; Bansal, Manisha ; Becker, Maximilian T. ; Bakhit, Babak ; Maity, Tuhin and Monserrat, Bartomeu , et al. (2024) In Advanced Materials 36(45).
Abstract

The discovery of ferroelectricity in nanoscale hafnia-based oxide films has spurred interest in understanding their emergent properties. Investigation focuses on the size-dependent polarization behavior, which is sensitive to content and movement of oxygen vacancies. Though polarization switching and electrochemical reactions is shown to co-occur, their relationship remains unclear. This study employs X-ray photoelectron spectroscopy with depth sensitivity to examine changes in electrochemical states occurring during polarization switching. Contrasting Hf0.5Zr0.5O2 (HZO) with Hf0.88La0.04Ta0.08O2 (HLTO), a composition with an equivalent structure and comparable... (More)

The discovery of ferroelectricity in nanoscale hafnia-based oxide films has spurred interest in understanding their emergent properties. Investigation focuses on the size-dependent polarization behavior, which is sensitive to content and movement of oxygen vacancies. Though polarization switching and electrochemical reactions is shown to co-occur, their relationship remains unclear. This study employs X-ray photoelectron spectroscopy with depth sensitivity to examine changes in electrochemical states occurring during polarization switching. Contrasting Hf0.5Zr0.5O2 (HZO) with Hf0.88La0.04Ta0.08O2 (HLTO), a composition with an equivalent structure and comparable average ionic radius, electrochemical states are directly observed for specific polarization directions. Lower-polarization films exhibit more significant electrochemical changes upon switching, suggesting an indirect relationship between polarization and electrochemical state. This research illuminates the complex interplay between polarization and electrochemical dynamics, providing evidence for intrinsic polar states in HfO2-based ferroelectrics.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
electrochemistry, ferroelectricity, hafnia, x-ray photoelectron spectroscopy
in
Advanced Materials
volume
36
issue
45
article number
2408572
publisher
John Wiley & Sons Inc.
external identifiers
  • scopus:85203688242
  • pmid:39263830
ISSN
0935-9648
DOI
10.1002/adma.202408572
language
English
LU publication?
yes
additional info
Publisher Copyright: © 2024 The Author(s). Advanced Materials published by Wiley-VCH GmbH.
id
869fd3be-5715-4a10-8f84-409983149d27
date added to LUP
2024-12-09 14:33:14
date last changed
2024-12-10 11:12:18
@article{869fd3be-5715-4a10-8f84-409983149d27,
  abstract     = {{<p>The discovery of ferroelectricity in nanoscale hafnia-based oxide films has spurred interest in understanding their emergent properties. Investigation focuses on the size-dependent polarization behavior, which is sensitive to content and movement of oxygen vacancies. Though polarization switching and electrochemical reactions is shown to co-occur, their relationship remains unclear. This study employs X-ray photoelectron spectroscopy with depth sensitivity to examine changes in electrochemical states occurring during polarization switching. Contrasting Hf<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2</sub> (HZO) with Hf<sub>0.88</sub>La<sub>0.04</sub>Ta<sub>0.08</sub>O<sub>2</sub> (HLTO), a composition with an equivalent structure and comparable average ionic radius, electrochemical states are directly observed for specific polarization directions. Lower-polarization films exhibit more significant electrochemical changes upon switching, suggesting an indirect relationship between polarization and electrochemical state. This research illuminates the complex interplay between polarization and electrochemical dynamics, providing evidence for intrinsic polar states in HfO<sub>2</sub>-based ferroelectrics.</p>}},
  author       = {{Hill, Megan O. and Kim, Ji Soo and Müller, Moritz L. and Phuyal, Dibya and Taper, Sunil and Bansal, Manisha and Becker, Maximilian T. and Bakhit, Babak and Maity, Tuhin and Monserrat, Bartomeu and Martino, Giuliana Di and Strkalj, Nives and MacManus-Driscoll, Judith L.}},
  issn         = {{0935-9648}},
  keywords     = {{electrochemistry; ferroelectricity; hafnia; x-ray photoelectron spectroscopy}},
  language     = {{eng}},
  month        = {{11}},
  number       = {{45}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Advanced Materials}},
  title        = {{Depth-Resolved X-Ray Photoelectron Spectroscopy Evidence of Intrinsic Polar States in HfO<sub>2</sub>-Based Ferroelectrics}},
  url          = {{http://dx.doi.org/10.1002/adma.202408572}},
  doi          = {{10.1002/adma.202408572}},
  volume       = {{36}},
  year         = {{2024}},
}