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<p>Hafnia-based ferroelectric materials have garnered considerable attention due to robust ferroelectricity in ultrathin films and excellent compatibility with silicon-based technology. Theoretical predictions of the polarization along [001] direction of ferroelectric HfO<sub>2</sub> are 50 μC/cm<sup>2</sup> and 70 μC/cm<sup>2</sup>, respectively, depending on the switching mechanism. However, most experimental observations of the intrinsic polarization are much lower than these predictions. Here, we report that an intrinsic remnant polarization up to 40 μC/cm<sup>2</sup> is achieved in epitaxially grown (111)-oriented Hf<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2</sub>/Hf<sub>0.9</sub>La<sub>0.1</sub>O<sub>2</sub> multilayer film, corresponding to 69.3 μC/cm<sup>2</sup> along [001], approaching the theoretical limit. Structural analyses reveal a rhombohedral-distorted orthorhombic phase in the Hf<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2</sub>/Hf<sub>0.9</sub>La<sub>0.1</sub>O<sub>2</sub> multilayers, stabilized by an in-plane compressive strain. Density functional theory calculations demonstrate that La doping in Hf<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2</sub>/Hf<sub>0.9</sub>La<sub>0.1</sub>O<sub>2</sub> promotes an unconventional switching pathway and contributes to the high intrinsic polarization. These findings provide a compelling strategy for achieving high intrinsic polarization and establish a design paradigm for high-performance hafnia-based ferroelectric devices.</p>

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Approaching theoretical polarization limit in HfZrO2/HfLaO2 multilayers

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月24日

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  • Shu Shi,
  • Haolong Xi,
  • Hanxin Su,
  • Fatoye Sawyerr,
  • Zhongran Liu,
  • Zekun Zhang,
  • Geng Huangfu,
  • Jiangzhen Niu,
  • Yiyuan Sun,
  • Ping Yang,
  • Xiao Gong,
  • Wei Chen,
  • Evgeny Y. Tsymbal,
  • Xiaobing Yan,
  • He Tian,
  • Tengfei Cao,
  • Jingsheng Chen

摘要

Hafnia-based ferroelectric materials have garnered considerable attention due to robust ferroelectricity in ultrathin films and excellent compatibility with silicon-based technology. Theoretical predictions of the polarization along [001] direction of ferroelectric HfO2 are 50 μC/cm2 and 70 μC/cm2, respectively, depending on the switching mechanism. However, most experimental observations of the intrinsic polarization are much lower than these predictions. Here, we report that an intrinsic remnant polarization up to 40 μC/cm2 is achieved in epitaxially grown (111)-oriented Hf0.5Zr0.5O2/Hf0.9La0.1O2 multilayer film, corresponding to 69.3 μC/cm2 along [001], approaching the theoretical limit. Structural analyses reveal a rhombohedral-distorted orthorhombic phase in the Hf0.5Zr0.5O2/Hf0.9La0.1O2 multilayers, stabilized by an in-plane compressive strain. Density functional theory calculations demonstrate that La doping in Hf0.5Zr0.5O2/Hf0.9La0.1O2 promotes an unconventional switching pathway and contributes to the high intrinsic polarization. These findings provide a compelling strategy for achieving high intrinsic polarization and establish a design paradigm for high-performance hafnia-based ferroelectric devices.