Interface-engineered ferroelectricity of epitaxial Hf0.5Zr0.5O2 thin films

Shu Shi, Haolong Xi, Tengfei Cao, Weinan Lin, Zhongran Liu, Jiangzhen Niu, Da Lan, Chenghang Zhou, Jing Cao, Hanxin Su, Tieyang Zhao, Ping Yang, Yao Zhu, Xiaobing Yan (), Evgeny Y. Tsymbal (), He Tian () and Jingsheng Chen ()
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Shu Shi: National University of Singapore
Haolong Xi: Electron Microscopy Centre of Lanzhou University and Key Laboratory of Magnetism and Magnetic Materials of the Ministry of Education, Lanzhou University
Tengfei Cao: University of Nebraska
Weinan Lin: Xiamen University
Zhongran Liu: Zhejiang University
Jiangzhen Niu: Hebei University
Da Lan: National University of Singapore
Chenghang Zhou: National University of Singapore
Jing Cao: Technology and Research (A*STAR)
Hanxin Su: National University of Singapore
Tieyang Zhao: National University of Singapore
Ping Yang: National University of Singapore
Yao Zhu: Technology and Research (A*STAR)
Xiaobing Yan: Hebei University
Evgeny Y. Tsymbal: University of Nebraska
He Tian: Zhejiang University
Jingsheng Chen: National University of Singapore

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: Abstract Ferroelectric hafnia-based thin films have attracted intense attention due to their compatibility with complementary metal-oxide-semiconductor technology. However, the ferroelectric orthorhombic phase is thermodynamically metastable. Various efforts have been made to stabilize the ferroelectric orthorhombic phase of hafnia-based films such as controlling the growth kinetics and mechanical confinement. Here, we demonstrate a key interface engineering strategy to stabilize and enhance the ferroelectric orthorhombic phase of the Hf0.5Zr0.5O2 thin film by deliberately controlling the termination of the bottom La0.67Sr0.33MnO3 layer. We find that the Hf0.5Zr0.5O2 films on the MnO2-terminated La0.67Sr0.33MnO3 have more ferroelectric orthorhombic phase than those on the LaSrO-terminated La0.67Sr0.33MnO3, while with no wake-up effect. Even though the Hf0.5Zr0.5O2 thickness is as thin as 1.5 nm, the clear ferroelectric orthorhombic (111) orientation is observed on the MnO2 termination. Our transmission electron microscopy characterization and theoretical modelling reveal that reconstruction at the Hf0.5Zr0.5O2/ La0.67Sr0.33MnO3 interface and hole doping of the Hf0.5Zr0.5O2 layer resulting from the MnO2 interface termination are responsible for the stabilization of the metastable ferroelectric phase of Hf0.5Zr0.5O2. We anticipate that these results will inspire further studies of interface-engineered hafnia-based systems.

Date: 2023
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DOI: 10.1038/s41467-023-37560-3

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