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<p>The ferroelectricity in nanoscale HfO<sub>2</sub>-based films enables their applications more promising than that of the perovskite oxides, taking into account the easy compatibility with the modern silicon-based semiconductor technology. However, the well-known polar orthorhombic phase is thermodynamically metastable, making the applications of HfO<sub>2</sub>-based ferroelectrics challenging in terms of uncontrollability and consequently instability of the physical performance in electronic devices. Here we report the robust ferroelectricity in stable monoclinic Hf<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2</sub> single-crystalline films, which was known as non-polar before. The as-prepared films display high endurance performance of wake-up free and non-fatigue behavior up to 10<sup>12</sup> cycles. Multimode imaging under aberration-corrected scanning transmission electron microscopy reveals that such an unexpected ferroelectric behavior is resultant from an antiphase boundaries-derived monoclinic polar variant (space group, <i>Pc</i>) intergrown with the nonpolar monoclinic phase (<i>P2</i><sub><i>1</i></sub><i>/c</i>). The switching barrier for the stable polar variant is only 20~50% of that for the metastable orthorhombic phase according to the calculation by the nudged elastic band method. These findings provide a practical approach for designing robust ferroelectricity in hafnia-based materials and would be helpful for the development of lower energy-cost and long-life memory devices compatible with integrated circuit technology.</p>

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A stable monoclinic variant and resultant robust ferroelectricity in single-crystalline hafnia-based films

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年10月3日

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  • Wan-Rong Geng,
  • Yu-Jia Wang,
  • Yin-Lian Zhu,
  • Sirui Zhang,
  • Huiqin Ma,
  • Yun-Long Tang,
  • Shi Tuo,
  • Xiu-Liang Ma

摘要

The ferroelectricity in nanoscale HfO2-based films enables their applications more promising than that of the perovskite oxides, taking into account the easy compatibility with the modern silicon-based semiconductor technology. However, the well-known polar orthorhombic phase is thermodynamically metastable, making the applications of HfO2-based ferroelectrics challenging in terms of uncontrollability and consequently instability of the physical performance in electronic devices. Here we report the robust ferroelectricity in stable monoclinic Hf0.5Zr0.5O2 single-crystalline films, which was known as non-polar before. The as-prepared films display high endurance performance of wake-up free and non-fatigue behavior up to 1012 cycles. Multimode imaging under aberration-corrected scanning transmission electron microscopy reveals that such an unexpected ferroelectric behavior is resultant from an antiphase boundaries-derived monoclinic polar variant (space group, Pc) intergrown with the nonpolar monoclinic phase (P21/c). The switching barrier for the stable polar variant is only 20~50% of that for the metastable orthorhombic phase according to the calculation by the nudged elastic band method. These findings provide a practical approach for designing robust ferroelectricity in hafnia-based materials and would be helpful for the development of lower energy-cost and long-life memory devices compatible with integrated circuit technology.