Evolution of the conductive filament system in HfO2-based memristors observed by direct atomic-scale imaging

Ying Zhang, Ge-Qi Mao, Xiaolong Zhao (), Yu Li, Meiyun Zhang, Zuheng Wu, Wei Wu, Huajun Sun, Yizhong Guo, Lihua Wang, Xumeng Zhang, Qi Liu, Hangbing Lv, Kan-Hao Xue (), Guangwei Xu, Xiangshui Miao, Shibing Long () and Ming Liu ()
Additional contact information
Ying Zhang: Key Laboratory of Microelectronic Devices & Integration Technology, Institute of Microelectronics of Chinese Academy of Sciences
Ge-Qi Mao: Huazhong University of Science and Technology
Xiaolong Zhao: University of Science and Technology of China
Yu Li: Key Laboratory of Microelectronic Devices & Integration Technology, Institute of Microelectronics of Chinese Academy of Sciences
Meiyun Zhang: Key Laboratory of Microelectronic Devices & Integration Technology, Institute of Microelectronics of Chinese Academy of Sciences
Zuheng Wu: Key Laboratory of Microelectronic Devices & Integration Technology, Institute of Microelectronics of Chinese Academy of Sciences
Wei Wu: Huazhong University of Science and Technology
Huajun Sun: Huazhong University of Science and Technology
Yizhong Guo: Beijing University of Technology
Lihua Wang: Beijing University of Technology
Xumeng Zhang: Key Laboratory of Microelectronic Devices & Integration Technology, Institute of Microelectronics of Chinese Academy of Sciences
Qi Liu: Key Laboratory of Microelectronic Devices & Integration Technology, Institute of Microelectronics of Chinese Academy of Sciences
Hangbing Lv: Key Laboratory of Microelectronic Devices & Integration Technology, Institute of Microelectronics of Chinese Academy of Sciences
Kan-Hao Xue: Huazhong University of Science and Technology
Guangwei Xu: University of Science and Technology of China
Xiangshui Miao: Huazhong University of Science and Technology
Shibing Long: University of Science and Technology of China
Ming Liu: Key Laboratory of Microelectronic Devices & Integration Technology, Institute of Microelectronics of Chinese Academy of Sciences

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract The resistive switching effect in memristors typically stems from the formation and rupture of localized conductive filament paths, and HfO2 has been accepted as one of the most promising resistive switching materials. However, the dynamic changes in the resistive switching process, including the composition and structure of conductive filaments, and especially the evolution of conductive filament surroundings, remain controversial in HfO2-based memristors. Here, the conductive filament system in the amorphous HfO2-based memristors with various top electrodes is revealed to be with a quasi-core-shell structure consisting of metallic hexagonal-Hf6O and its crystalline surroundings (monoclinic or tetragonal HfOx). The phase of the HfOx shell varies with the oxygen reservation capability of the top electrode. According to extensive high-resolution transmission electron microscopy observations and ab initio calculations, the phase transition of the conductive filament shell between monoclinic and tetragonal HfO2 is proposed to depend on the comprehensive effects of Joule heat from the conductive filament current and the concentration of oxygen vacancies. The quasi-core-shell conductive filament system with an intrinsic barrier, which prohibits conductive filament oxidation, ensures the extreme scalability of resistive switching memristors. This study renovates the understanding of the conductive filament evolution in HfO2-based memristors and provides potential inspirations to improve oxide memristors for nonvolatile storage-class memory applications.

Date: 2021
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DOI: 10.1038/s41467-021-27575-z

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