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

Wan-Rong Geng, Yu-Jia Wang, Yin-Lian Zhu, Sirui Zhang, Huiqin Ma, Yun-Long Tang, Shi Tuo and Xiu-Liang Ma ()
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Wan-Rong Geng: Songshan Lake Materials Laboratory
Yu-Jia Wang: Chinese Academy of Sciences
Yin-Lian Zhu: Songshan Lake Materials Laboratory
Sirui Zhang: Xidian University
Huiqin Ma: Zhejiang Laboratory
Yun-Long Tang: Chinese Academy of Sciences
Shi Tuo: Zhejiang Laboratory
Xiu-Liang Ma: Songshan Lake Materials Laboratory

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract 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.

Date: 2025
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DOI: 10.1038/s41467-025-63907-z

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