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Unlocking the phase evolution of the hidden non-polar to ferroelectric transition in HfO2-based bulk crystals

Author

Listed:
  • Shuxian Wang

    (Shandong University)

  • Yihao Shen

    (Shandong University)

  • Xiaoyu Yang

    (Anhui University)

  • Pengfei Nan

    (Anhui University)

  • Yuzhou He

    (Anhui University)

  • Ning Lu

    (Shandong University)

  • Haohai Yu

    (Shandong University)

  • Binghui Ge

    (Anhui University)

  • Shujun Zhang

    (University of Wollongong)

  • Huaijin Zhang

    (Shandong University)

Abstract

The discovery of ferroelectricity in hafnium dioxide (HfO2) thin films over the past decade has revolutionized the landscape of ferroelectrics, providing a promising candidate for next-generation ferroelectrics beyond the constraints of Moore’s law. However, the underlying formation mechanism of their metastable and volatile ferroelectric phase is under debate. Herein, we successfully grow HfO2-based (Lu:Hf1−xZrxO2) bulk crystals and gain a comprehensive understanding of the non-polar to ferroelectric phase evolution. We achieve a controllable polymorphic engineering by elucidating the synergistic modulation of co-doped Lu3+ and Zr4+ ions. Our investigation unveils the intricate local structural transitions involved in the formation of the ferroelectric orthorhombic Pbc21 phase from the metastable tetragonal phase. We also establish a controllable tetragonal-to-orthorhombic transformation route, effectively improving the ferroelectric phase component within bulk crystals. Our findings will advance the comprehension of ferroelectric mechanisms in fluorite-structured materials, paving the way for significant strides in developing HfO2-based nonvolatile electronic and photonic devices.

Suggested Citation

  • Shuxian Wang & Yihao Shen & Xiaoyu Yang & Pengfei Nan & Yuzhou He & Ning Lu & Haohai Yu & Binghui Ge & Shujun Zhang & Huaijin Zhang, 2025. "Unlocking the phase evolution of the hidden non-polar to ferroelectric transition in HfO2-based bulk crystals," Nature Communications, Nature, vol. 16(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-59018-4
    DOI: 10.1038/s41467-025-59018-4
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    References listed on IDEAS

    as
    1. Qing Luo & Yan Cheng & Jianguo Yang & Rongrong Cao & Haili Ma & Yang Yang & Rong Huang & Wei Wei & Yonghui Zheng & Tiancheng Gong & Jie Yu & Xiaoxin Xu & Peng Yuan & Xiaoyan Li & Lu Tai & Haoran Yu & , 2020. "A highly CMOS compatible hafnia-based ferroelectric diode," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    2. Suraj S. Cheema & Nirmaan Shanker & Li-Chen Wang & Cheng-Hsiang Hsu & Shang-Lin Hsu & Yu-Hung Liao & Matthew San Jose & Jorge Gomez & Wriddhi Chakraborty & Wenshen Li & Jong-Ho Bae & Steve K. Volkman , 2022. "Ultrathin ferroic HfO2–ZrO2 superlattice gate stack for advanced transistors," Nature, Nature, vol. 604(7904), pages 65-71, April.
    3. Yan Cheng & Zhaomeng Gao & Kun Hee Ye & Hyeon Woo Park & Yonghui Zheng & Yunzhe Zheng & Jianfeng Gao & Min Hyuk Park & Jung-Hae Choi & Kan-Hao Xue & Cheol Seong Hwang & Hangbing Lyu, 2022. "Reversible transition between the polar and antipolar phases and its implications for wake-up and fatigue in HfO2-based ferroelectric thin film," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    4. Bethany M. Hudak & Sean W. Depner & Gregory R. Waetzig & Anjana Talapatra & Raymundo Arroyave & Sarbajit Banerjee & Beth S. Guiton, 2017. "Real-time atomistic observation of structural phase transformations in individual hafnia nanorods," Nature Communications, Nature, vol. 8(1), pages 1-9, August.
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