Hf0.5Zr0.5O2-ZrO2超晶格薄膜中铁电畴的电子束辐照响应行为研究

Hf_0.5Zr_0.5O₂-ZrO₂超晶格薄膜中铁电畴的电子束辐照响应行为研究

王博锐^1，2，耿皖荣^1*，朱银莲¹，张思瑞²，马秀良^1，3，4*

(1.松山湖材料实验室大湾区显微科学与技术研究中心，广东 东莞 523808；2.西安电子科技大学 先进材料与纳米科技学院，陕西 西安 710126；3.中国科学院物理研究所，北京 100190；4.粤港澳大湾区量子科学中心，广东 深圳 518000)

摘　要　　铪基铁电薄膜因其优异的工艺兼容性和可扩展性优势，被视为突破摩尔定律极限的新一代铁电候选材料。然而，其核心物理机制——尤其是极化翻转动力学与畴结构演变规律——仍存在认知空白。本研究通过原位像差校正透射电子显微技术，系统揭示了外延Hf_0.5Zr_0.5O₂-ZrO₂超晶格薄膜在电子束辐照作用下的原子尺度结构演化规律。基于原子分辨的扫描透射电镜（scanning transmission electron microscopy，STEM）的多种成像模式的表征发现，电子束辐照可在Hf_0.5Zr_0.5O₂-ZrO₂层内诱导产生单胞尺度的极化错排畴，该中间态结构具有自发恢复特性。另外，电子束辐照可触发单畴体系向含180°带电畴壁的双畴态可逆转变，且畴壁两侧极化区域表现出独立翻转特性。本研究首次实现了铪基铁电极化的单胞级精准操控，从原子尺度揭示了极化翻转与畴壁动力学的微观机制，为开发高密度非易失性铁电存储器提供了重要的理论依据。

关键词　　铪基铁电超晶格；电子束辐照；畴结构演变；像差校正透射电子显微镜

中图分类号：TB34；TB383；TG115.21⁺5.3    文献标识码：A Doi:10.3969/j.issn.1000-6281.2025.05.004

Response behavior of ferroelectric domains to electron beam irradiation in Hf_0.5Zr_0.5O₂-ZrO₂ superlattice thin films

WANG Borui^1，2，GENG Wanrong^1*，ZHU Yinlian¹，ZHANG Sirui²，MA Xiuliang^1，3，4*

(1.Bay Area Center for Electron Microscopy，Songshan Lake Materials Laboratory，Dongguan Guangdong 523808；2.School of Advanced Materials and Nanotechnology，Xidian University，Xi'an Shanxi 710126；3.Institute of Physics，Chinese Academy of Sciences，Beijing 100190；4.Quantum Science Center of Guangdong-HongKong-Macau Greater Bay Area，Shenzhen Guangdong 518000, China)

Abstract　　Hafnium-based ferroelectric thin films are considered as promising next-generation candidate materials for surpassing Moore's Law limitations due to their excellent process compatibility and scalability. However, the fundamental physical mechanisms—particularly those governing polarization switching dynamics and domain structure evolution—remain poorly understood. This study systematically investigates the atomic-scale structural evolution of epitaxial Hf_0.5Zr_0.5O₂-ZrO₂ superlattice thin films under electron beam irradiation using in situ aberration-corrected transmission electron microscopy. Atomic-resolution scanning transmission electron microscopy (STEM) imaging revealed that electron beam irradiation induced polarization-misaligned domains at the unit-cell scale within the Hf_0.5Zr_0.5O₂-ZrO₂ layers. These intermediate metastable structures exhibited spontaneous recovery behavior. Additionally, electron beam irradiation reversibly transformed a single-domain system into a two-domain state containing 180° charged domain walls, with the polarized regions on both sides of the domain walls exhibiting independent switching behavior. This work achieves unit-cell-level precision in manipulating polarization in hafnium-based ferroelectric for the first time, uncovering the microscopic mechanisms of polarization switching and domain wall dynamics at the atomic scale. The findings provide critical theoretical foundations for developing high-density nonvolatile ferroelectric memory devices.

Keywords　　hafnium-based ferroelectric superlattice; electron beam irradiation; evolution of domain structure; aberration-corrected transmission electron microscope

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