Wang Shuxian, Shen Yihao, Yang Xiaoyu, Nan Pengfei, He Yuzhou, Lu Ning, Yu Haohai, Ge Binghui, Zhang Shujun, Zhang Huaijin
State Key Laboratory of Crystal Materials and School of Crystal Materials, Shandong University, Jinan, China.
Information Materials and Intelligent Sensing Laboratory of Anhui Province, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Institutes of Physical Science and Information Technology, Anhui University, Hefei, China.
Nat Commun. 2025 Apr 21;16(1):3745. doi: 10.1038/s41467-025-59018-4.
The discovery of ferroelectricity in hafnium dioxide (HfO) 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-based (Lu:HfZrO) 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 and Zr ions. Our investigation unveils the intricate local structural transitions involved in the formation of the ferroelectric orthorhombic Pbc2 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-based nonvolatile electronic and photonic devices.
在过去十年中，二氧化铪（HfO）薄膜中铁电现象的发现彻底改变了铁电体的格局，为超越摩尔定律限制的下一代铁电体提供了一个有前景的候选材料。然而，其亚稳且易挥发铁电相的潜在形成机制仍存在争议。在此，我们成功生长出基于HfO的（Lu:HfZrO）块状晶体，并全面了解了从非极性到铁电相的演变过程。通过阐明共掺杂Lu和Zr离子的协同调制作用，我们实现了可控的多晶型工程。我们的研究揭示了从亚稳四方相形成铁电正交Pbc2相所涉及的复杂局部结构转变。我们还建立了可控的四方相向正交相转变途径，有效提高了块状晶体中的铁电相组分。我们的发现将推动对萤石结构材料中铁电机制的理解，为基于HfO的非易失性电子和光子器件的重大进展铺平道路。
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