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<p>Complementary-metal-oxide-semiconductor-compatible HfO<sub>2</sub>-based high-<i>κ</i> dielectrics are pivotal for next-generation electronics in the post-Moore’s Law era. However, establishing coherent interfaces via morphotropic phase boundaries across the tetragonal and orthorhombic (ferroelectric or antiferroelectric) phases—a key strategy for enhancing dielectric properties—remains challenging due to unclear atomic-scale mechanisms and inherent thermal instability, which compromises long-term stability and reliability. To address this, we leverage metallurgical quenching principles to stabilize tetragonal/orthorhombic<i>-</i>antiferroelectric morphotropic phase boundaries in HfO<sub>2</sub>-based (Lu:Hf<sub>0.6</sub>Zr<sub>0.4</sub>O<sub>2</sub>) bulk crystals. Through precise composition tuning and growth optimization, we stabilize these metastable morphotropic phase boundaries at the tetragonal/orthorhombic<i>-</i>antiferroelectric interface at room temperature, achieving a comparable <i>κ</i>-value (57) to actively studied tetragonal/orthorhombic<i>-</i>ferroelectric counterparts. Microstructural characterization reveals how tensile strain within the <i>t</i>-phase drives dielectric enhancement through softening of the low-frequency <i>E</i><sub>u</sub> phonon mode. Critically, the tetragonal/orthorhombic<i>-</i>antiferroelectric morphotropic phase boundary demonstrates a ~58% reduction in <i>κ</i> variation rate over 30–200 °C relative to tetragonal/orthorhombic<i>-</i>ferroelectric counterparts, signifying superior thermal stability. Our study establishes a generalizable design paradigm for developing high-<i>κ</i> dielectrics in fluorite-structured materials, advancing next-generation complementary-metal-oxide-semiconductor-compatible-integrated functional devices for data storage, energy harvesting, sensing, and integrated photonics.</p>

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Atomic-scale mechanism unlocks thermal-stable high-κ performance in HfO2 via coherent interfaces

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月16日

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  • Yihao Shen,
  • Hongzheng Wang,
  • Xiaochun Ma,
  • Yuxiao Liu,
  • Fei Liang,
  • Shuxian Wang,
  • Pengfei Nan,
  • Binghui Ge,
  • Shujun Zhang,
  • Haohai Yu,
  • Huaijin Zhang

摘要

Complementary-metal-oxide-semiconductor-compatible HfO2-based high-κ dielectrics are pivotal for next-generation electronics in the post-Moore’s Law era. However, establishing coherent interfaces via morphotropic phase boundaries across the tetragonal and orthorhombic (ferroelectric or antiferroelectric) phases—a key strategy for enhancing dielectric properties—remains challenging due to unclear atomic-scale mechanisms and inherent thermal instability, which compromises long-term stability and reliability. To address this, we leverage metallurgical quenching principles to stabilize tetragonal/orthorhombic-antiferroelectric morphotropic phase boundaries in HfO2-based (Lu:Hf0.6Zr0.4O2) bulk crystals. Through precise composition tuning and growth optimization, we stabilize these metastable morphotropic phase boundaries at the tetragonal/orthorhombic-antiferroelectric interface at room temperature, achieving a comparable κ-value (57) to actively studied tetragonal/orthorhombic-ferroelectric counterparts. Microstructural characterization reveals how tensile strain within the t-phase drives dielectric enhancement through softening of the low-frequency Eu phonon mode. Critically, the tetragonal/orthorhombic-antiferroelectric morphotropic phase boundary demonstrates a ~58% reduction in κ variation rate over 30–200 °C relative to tetragonal/orthorhombic-ferroelectric counterparts, signifying superior thermal stability. Our study establishes a generalizable design paradigm for developing high-κ dielectrics in fluorite-structured materials, advancing next-generation complementary-metal-oxide-semiconductor-compatible-integrated functional devices for data storage, energy harvesting, sensing, and integrated photonics.