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<p>Understanding ferroelectric phase stability in hafnium-based oxides is crucial for high-quality thin-film fabrication and device applications. Multiple strategies stabilize the phase, with evidence highlighting extra holes’ key role. However, research on extra holes’ impact on ferroelectric phase stabilization remains inadequate. This study combines first-principles calculations with experimental data, identifying a critical extra-hole concentration threshold (0.3 h/f.u.) for HfO<sub>2</sub> ferroelectric phase stabilization. We designed two coordinated experiments to verify the extra-hole threshold in HfO<sub>2</sub>. Using SrRuO<sub>3</sub> (SRO) as the bottom electrode, we studied three HfO<sub>2</sub> systems (Sm, Eu, and La doped). All systems showed optimal ferroelectric performance at 7.5% doping. Our results also showed that HfO<sub>2</sub> films on Sm-doped (La<sub>0.67</sub>Sr<sub>0.33</sub>MnO<sub>3</sub>) LSMO (5.5% doping) achieve optimal polarization, comparable to SRO (7.5%). These mutually corroborative experimental and theoretical results indicate that the extra-hole threshold optimizes HfO<sub>2</sub> ferroelectric thin film growth and facilitates its electronic device applications.</p>

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Extra hole threshold in HfO2 ferroelectric phase stabilization

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月24日

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  • Xixiang Jing,
  • Yuhao Yue,
  • Shuning Lv,
  • Kang Jia,
  • Kepeng Song,
  • Fatoye Sawyerr,
  • Qi Hu,
  • Zekun Zhang,
  • Shu Shi,
  • Shifeng Wen,
  • Li-Min Liu,
  • Jingsheng Chen,
  • Xiaoli Fan,
  • Zheng Wen,
  • Tengfei Cao

摘要

Understanding ferroelectric phase stability in hafnium-based oxides is crucial for high-quality thin-film fabrication and device applications. Multiple strategies stabilize the phase, with evidence highlighting extra holes’ key role. However, research on extra holes’ impact on ferroelectric phase stabilization remains inadequate. This study combines first-principles calculations with experimental data, identifying a critical extra-hole concentration threshold (0.3 h/f.u.) for HfO2 ferroelectric phase stabilization. We designed two coordinated experiments to verify the extra-hole threshold in HfO2. Using SrRuO3 (SRO) as the bottom electrode, we studied three HfO2 systems (Sm, Eu, and La doped). All systems showed optimal ferroelectric performance at 7.5% doping. Our results also showed that HfO2 films on Sm-doped (La0.67Sr0.33MnO3) LSMO (5.5% doping) achieve optimal polarization, comparable to SRO (7.5%). These mutually corroborative experimental and theoretical results indicate that the extra-hole threshold optimizes HfO2 ferroelectric thin film growth and facilitates its electronic device applications.