Enhancing ferroelectric stability: wide-range of adaptive control in epitaxial HfO2/ZrO2 superlattices

Abstract

The metastability of the polar phase in HfO₂, despite its excellent compatibility with the complementary metal-oxide-semiconductor process, remains a key obstacle for its industrial applications. Traditional stabilization approaches, such as doping, often induce crystal defects and impose constraints on the thickness of ferroelectric HfO₂ thin films. These limitations render the ferroelectric properties vulnerable to degradation, particularly due to phase transitions under operational conditions. Here, we demonstrate robust ferroelectricity in high-quality epitaxial (HfO₂)_n/(ZrO₂)_n superlattices, which exhibit significantly enhanced ferroelectric stability across an extended thickness range. Optimized-period superlattices maintain stable ferroelectricity from up to 100 nm, excellent fatigue resistance exceeding 10⁹ switching cycles, and a low coercive field of ~0.85 MV/cm. First-principles calculations reveal that the kinetic energy barrier of phase transition and interfacial formation energy are crucial factors in suppressing the formation of non-polar phases. This work establishes a versatile platform for exploring high-performance fluorite-structured superlattices and advances the integration of HfO₂-based ferroelectrics into a broader range of applications.