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

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

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-59018-4

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