Unraveling the Effects of Depolarization in Ultrathin Barium Titanate
7 affiliations
- 1Department of Materials Science and Engineering University of California Berkeley California USA
- 2Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley California USA
- 3Rice Advanced Materials Institute Rice University Houston Texas USA
- 4Advanced Light Source Lawrence Berkeley National Laboratory Berkeley California USA
- 5National Synchrotron Light Source II Brookhaven National Laboratory Upton New York USA
- 6Applied Mathematics and Computational Research Division Lawrence Berkeley National Laboratory Berkeley California USA
- 7Departments of Materials Science and NanoEngineering Chemistry, and Physics and Astronomy Rice University Houston Texas USA
Abstract
Depolarization fields pose a critical obstacle to realizing ultrathin ferroelectric devices with low‐voltage operation. Although the phenomenology of depolarization has been observed for decades, whether polarization loss proceeds through suppression of ferroelectric order or reverse‐domain formation has remained unresolved. Here, a combination of experiment and simulation resolves this question and establishes the electrostatic origin of polarization instability in the ultrathin limit for BaTiO3. Synchrotron X‐ray absorption spectroscopy confirms that the polar structural distortion in BaTiO3 persists down to (at least) 3 nm even as the remanent polarization falls sharply, identifying reverse‐domain formation as the primary mechanism of polarization loss. Time‐resolved pulsed‐switching measurements reveal dynamically evolving depolarization fields that converge to a thickness‐independent equilibrium value. An electrostatic model attributes these fields to the effective series capacitance of the electrode interfaces, validated through thickness scaling and dielectric‐buffer experiments. Phase‐field simulations reveal that modifying this series capacitance reshapes switching dynamics by redistributing internal fields without altering the intrinsic ferroelectric energy landscape. Defects play a consequential secondary role, independently controlling relaxation pathways within this electrostatically constrained regime. These results establish depolarization as a system‐level effect governed by heterostructure boundary conditions, and identify interfacial design and defect management as complementary strategies for stabilizing polarization in ultrathin ferroelectrics.
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BibTeX
@article{lee2026unraveling,
title = {{Unraveling the Effects of Depolarization in Ultrathin Barium Titanate}},
author = {Thomas Lee and Prabhat Kumar and Christoph Klewe and Pravin Kavle and Padraic Shafer and Zhi (Jackie) Yao and Lane W. Martin},
journal = {Advanced Science},
year = {2026},
month = oct,
doi = {10.1002/advs.78103},
url = {https://doi.org/10.1002/advs.78103},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Unraveling the Effects of Depolarization in Ultrathin Barium Titanate
AU - Thomas Lee
AU - Prabhat Kumar
AU - Christoph Klewe
AU - Pravin Kavle
AU - Padraic Shafer
AU - Zhi (Jackie) Yao
AU - Lane W. Martin
PY - 2026
DA - 2026/10/31
JO - Advanced Science
DO - 10.1002/advs.78103
UR - https://doi.org/10.1002/advs.78103
AB - Depolarization fields pose a critical obstacle to realizing ultrathin ferroelectric devices with low‐voltage operation. Although the phenomenology of depolarization has been observed for decades, whether polarization loss proceeds through suppression of ferroelectric order or reverse‐domain formation has remained unresolved. Here, a combination of experiment and simulation resolves this question and establishes the electrostatic origin of polarization instability in the ultrathin limit for BaTiO3. Synchrotron X‐ray absorption spectroscopy confirms that the polar structural distortion in BaTiO3 persists down to (at least) 3 nm even as the remanent polarization falls sharply, identifying reverse‐domain formation as the primary mechanism of polarization loss. Time‐resolved pulsed‐switching measurements reveal dynamically evolving depolarization fields that converge to a thickness‐independent equilibrium value. An electrostatic model attributes these fields to the effective series capacitance of the electrode interfaces, validated through thickness scaling and dielectric‐buffer experiments. Phase‐field simulations reveal that modifying this series capacitance reshapes switching dynamics by redistributing internal fields without altering the intrinsic ferroelectric energy landscape. Defects play a consequential secondary role, independently controlling relaxation pathways within this electrostatically constrained regime. These results establish depolarization as a system‐level effect governed by heterostructure boundary conditions, and identify interfacial design and defect management as complementary strategies for stabilizing polarization in ultrathin ferroelectrics.
SN - 2198-3844
ER -