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<p>The discovery of ferroelectricity in hafnium dioxide (HfO<sub>2</sub>) 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 HfO<sub>2</sub>-based (Lu:Hf<sub>1−<i>x</i></sub>Zr<sub><i>x</i></sub>O<sub>2</sub>) 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 Lu<sup>3+</sup> and Zr<sup>4+</sup> ions. Our investigation unveils the intricate local structural transitions involved in the formation of the ferroelectric orthorhombic <i>Pbc</i>2<sub>1</sub> 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 HfO<sub>2</sub>-based nonvolatile electronic and photonic devices.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月21日

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  • Shuxian Wang,
  • Yihao Shen,
  • Xiaoyu Yang,
  • Pengfei Nan,
  • Yuzhou He,
  • Ning Lu,
  • Haohai Yu,
  • Binghui Ge,
  • Shujun Zhang,
  • Huaijin Zhang

摘要

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.