Engineering Grain Boundary Commensurability for Ferroelectric Stabilization in Hafnia-Based Films

Abstract

Grain boundaries fundamentally dictate the macroscopic properties of polycrystalline materials by breaking long-range symmetry. In ferroelectrics, these structural discontinuities are conventionally considered as detrimental features that induce depolarization fields and accumulate defects, thereby suppressing or pinning local polarization. Here, we demonstrate that the commensurability of grain boundaries inherently governs the polar-orthorhombic phase stability in polycrystalline Hf0.5Zr0.5O2 (HZO) thin films. Using depth-resolved multislice electron ptychography, we map the three-dimensional (3D) phase distribution across diverse boundaries with atomic resolution, revealing that highly commensurate grain boundaries effectively suppress the nonpolar-tetragonal phase by compensating for lattice mismatch while mitigating geometric frustration. Monte Carlo simulations uncover the atomistic and energetic origins of polar-phase stabilization, showing that commensurate grain boundaries favor the polar-orthorhombic phase more strongly than other grain boundaries. Guided by this principle, we epitaxially engineer HZO thin films to promote the preferential formation of commensurate grain boundaries, resulting in an approximately 60% enhancement in the remanent polarization of ferroelectric devices. These findings provide direct 3D experimental and theoretical evidence that establishes grain boundary commensurability as a critical degree of freedom for designing functional interfaces, guiding the construction of novel ceramics and polycrystalline ferroelectrics.

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BibTeX RIS

BibTeX

@misc{shi2026engineering,
  title = {{Engineering Grain Boundary Commensurability for Ferroelectric Stabilization in Hafnia-Based Films}},
  author = {Chuqiao Shi and Xinyan Li and Xing He and Kaiji Zhao and Jesse Schimpf and Akash Surampalli and Adan Mireles and Sergio Puebla and Yi Jiang and Ramamoorthy Ramesh and Xiaofeng Qian and Lane W. Martin and Andrew M. Rappe and Yimo Han},
  howpublished = {arXiv},
  year = {2026},
  month = sep,
  doi = {10.48550/arxiv.2609.39931},
  eprint = {2609.39931},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2609.39931},
}

RIS

TY  - UNPB
TI  - Engineering Grain Boundary Commensurability for Ferroelectric Stabilization in Hafnia-Based Films
AU  - Chuqiao Shi
AU  - Xinyan Li
AU  - Xing He
AU  - Kaiji Zhao
AU  - Jesse Schimpf
AU  - Akash Surampalli
AU  - Adan Mireles
AU  - Sergio Puebla
AU  - Yi Jiang
AU  - Ramamoorthy Ramesh
AU  - Xiaofeng Qian
AU  - Lane W. Martin
AU  - Andrew M. Rappe
AU  - Yimo Han
PY  - 2026
DA  - 2026/09/30
PB  - arXiv
DO  - 10.48550/arxiv.2609.39931
UR  - https://arxiv.org/abs/2609.39931
AB  - Grain boundaries fundamentally dictate the macroscopic properties of polycrystalline materials by breaking long-range symmetry. In ferroelectrics, these structural discontinuities are conventionally considered as detrimental features that induce depolarization fields and accumulate defects, thereby suppressing or pinning local polarization. Here, we demonstrate that the commensurability of grain boundaries inherently governs the polar-orthorhombic phase stability in polycrystalline Hf0.5Zr0.5O2 (HZO) thin films. Using depth-resolved multislice electron ptychography, we map the three-dimensional (3D) phase distribution across diverse boundaries with atomic resolution, revealing that highly commensurate grain boundaries effectively suppress the nonpolar-tetragonal phase by compensating for lattice mismatch while mitigating geometric frustration. Monte Carlo simulations uncover the atomistic and energetic origins of polar-phase stabilization, showing that commensurate grain boundaries favor the polar-orthorhombic phase more strongly than other grain boundaries. Guided by this principle, we epitaxially engineer HZO thin films to promote the preferential formation of commensurate grain boundaries, resulting in an approximately 60% enhancement in the remanent polarization of ferroelectric devices. These findings provide direct 3D experimental and theoretical evidence that establishes grain boundary commensurability as a critical degree of freedom for designing functional interfaces, guiding the construction of novel ceramics and polycrystalline ferroelectrics.
ER  -

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