光电协同调控下HfO<sub><i>x</i></sub>基阻变存储器的阻变特性

王英; 黄慧香; 黄香林; 郭婷婷

doi:10.7498/aps.72.20230797

摘要

利用磁控溅射法制备了Cu/HfO_x/Pt和Cu/HfO_x-ZnO/Pt器件. HfO_x器件和HfO_x-ZnO器件都表现出双极性阻变特性以及具有良好的保持性, 但HfO_x-ZnO器件具有更加优异的阻变性能, 例如均一性、耐受性和重复性. 研究表明, 通过增加ZnO富氧层有利于提高器件的阻变性能. 另外, HfO_x薄膜的禁带宽度约为5.10 eV, 对255 nm波长的光照没有响应. 而HfO_x-ZnO薄膜的禁带宽度减小为4.31 eV, 该器件在波长255 nm的光照作用下, 不仅可以提高器件的阻变性能, 还可以通过设置不同强度的光照使器件具有多级存储的能力. 研究发现, 器件在有无光照作用下的阻变行为都与薄膜中的氧空位有关, 所以本文提出了氧空位导电细丝物理模型来解释器件的阻变行为. 本文使用光电协同的方法为研制出低功耗、高存储密度的阻变存储器提供了新思路.

关键词:

Abstract

Cu/HfO_x/Pt and Cu/HfO_x-ZnO/Pt resistance random access memory (RRAM) devices are prepared by magnetron sputtering. The results show that the Cu/HfO_x/Pt device has the stable bipolar resistive switching characteristics, good retention (as long as 10⁴ s), and a switching ratio greater than 10³. The current conduction mechanism of HfO_x device is ohmic conduction at low resistance, while space charge limited current (SCLC) mechanism dominates at high resistance, and the conductive filament is composed of oxygen vacancies. Owing to the low content and random distribution of oxygen defects in the HfO_x film, the endurance and uniformity of the device are poor. Compared with HfO_x device, HfO_x-ZnO device exhibits lower operating voltage and better uniformity and stability. The main reason is that ZnO material has smaller formation energy of oxygen vacancy, which can produce more oxygen defects under electric field to participate in the resistive switching behavior of the device, thereby reducing the operating voltage and improving the uniformity of the device. In addition, owing to the existence of the interface between HfO_x and ZnO film, the random distribution of oxygen defects is inhibited, that is, the random fracture and formation of conductive filament are inhibited, which is beneficial to improving the uniformity of the device. In addition, the resistive switching behaviors of Cu/HfO_x/Pt and Cu/HfO_x-ZnO/Pt RRAM devices under different intensities of 255 nm ultraviolet illumination are studied. For Cu/HfO_x/Pt device, the light of 255 nm wavelength shows little effect on its resistive switching characteristics. For the Cu/HfO_x-ZnO/Pt RRAM device, the operating voltage and stability of the device can be improved by increasing the light intensity. Although the switching ratio of the device decreases with the increase of light intensity, the device can exhibit multiple resistance states by adjusting different light intensities to achieve multi-level storage. Finally, the analysis of the I-V curves of the devices indicates that the two types of devices show similar resistive switching mechanisms under the illumination of light or no light, which can be explained by the resistive switching mechanism of oxygen vacancy conductive filament. Therefore, a physical model based on the oxygen vacancy conductive filament is established to explain the resistive switching behavior of the device in this paper.

Keywords:

作者及机构信息

长安大学材料科学与工程学院, 西安　710061

通信作者: 郭婷婷, guott@chd.edu.cn

基金项目: 国家自然科学基金青年科学基金(批准号: 51802025)和陕西省自然科学基础研究计划(批准号: 2020JQ-384)资助的课题.

Authors and contacts

School of Materials Science and Engineering, Chang’an University, Xi’an 710061, China

Corresponding author: Guo Ting-Ting, guott@chd.edu.cn

Funds: Project supported by the Young Scientists Fund of the National Natural Science Foundation of China (Grant No. 51802025) and the Natural Science Foundation Research Plan of Shaanxi Province, China (Grant No. 2020JQ-384).

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参考文献

[1]	Guo T, Elshekh H, Yu Z, Yu B, Wang D, Kadhim M S, Chen Y Z, Hou W T, Sun B 2019 Mater. Today Commun. 20 100540 Google Scholar
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施引文献

图 1 HfO_x-ZnO样品的测试示意图(a)和TEM图像(b)

Fig. 1. Test schematic (a) and TEM images (b) of HfO_x-ZnO samples.

下载: 全尺寸图片幻灯片

图 2 (a), (b) HfO_x薄膜的XPS能谱; (c), (d) ZnO薄膜的XPS能谱

Fig. 2. (a), (b) XPS spectra of HfO_x film; (c), (d) XPS spectra of ZnO film.

下载: 全尺寸图片幻灯片

图 3 器件的双极性I-V曲线(插图为电形成过程)　(a) HfO_x; (b) HfO_x-ZnO

Fig. 3. Bipolar I-V curves of the device (Inset shows the forming process): (a) HfO_x; (b) HfO_x-ZnO.

下载: 全尺寸图片幻灯片

图 4 两种器件的阻变性能　(a)操作电压分布; (b)电阻分布; (c)耐受性; (d)保持性

Fig. 4. Switching properties of two samples: (a) Statistical distribution of switching voltages; (b) statistical distribution of resistances; (c) endurance; (d) retention properties.

下载: 全尺寸图片幻灯片

图 5 薄膜的UV-Vis光谱图(插图为光学带隙)　(a) HfO_x; (b) HfO_x-ZnO

Fig. 5. UV-Vis spectra of the films (Inset shows Tauc plot): (a) HfO_x; (b) HfO_x-ZnO.

下载: 全尺寸图片幻灯片

图 6 不同强度光照下器件的I-V曲线(插图为电形成过程)(a) HfO_x; (b) HfO_x-ZnO; (c) HfO_x-ZnO器件开启电压随光照强度的变化

Fig. 6. Bipolar I-V curves of the device under different light intensity: (The inset shows the forming process): (a) HfO_x; (b) HfO_x-ZnO; (c) forming voltage of HfO_x-ZnO device changes with the light intensity.

下载: 全尺寸图片幻灯片

图 7 HfO_x-ZnO器件不同强度光照下的阻变性能　(a)—(e)耐受性; (f)操作电压分布

Fig. 7. Resistive switching performance of the HfO_x-ZnO device under different light intensities: (a)–(e) Endurance; (f) statistical distribution of switching voltages.

下载: 全尺寸图片幻灯片

图 8 HfO_x-ZnO器件的多级存储的性能　(a)高低阻值; (b)保持性

Fig. 8. Multilevel memory performance of HfO_x-ZnO device: (a) High and low resistances; (b) retention properties.

下载: 全尺寸图片幻灯片

图 9 器件的阻变机制　(a) HfO_x; (b) HfO_x-ZnO; (c) Cu/HfO_x/Pt器件LRS阻值与温度的关系

Fig. 9. Resistive switching mechanism of devices: (a) HfO_x; (b) HfO_x-ZnO; (c) relationship between LRS resistance and temperature of Cu/HfO_x/Pt.

下载: 全尺寸图片幻灯片

图 10 HfO_x-ZnO器件的电阻开关物理微观过程

Fig. 10. Physical microscopic process of the resistance switch of the HfO_x-ZnO device.

下载: 全尺寸图片幻灯片

[1]	Guo T, Elshekh H, Yu Z, Yu B, Wang D, Kadhim M S, Chen Y Z, Hou W T, Sun B 2019 Mater. Today Commun. 20 100540 Google Scholar
[2]	Yoo S J, Agbenyeke R E, Choi H, Jeon K, Ryu J J, Eom T, Park B K, Chung T M, Jeong D S, Song W 2022 Appl. Surf. Sci. 577 151936 Google Scholar
[3]	Killedar S T, Ahir N A, Morankar P J, Tiwari A P, Kim D K 2020 Opt. Mater. 109 110333 Google Scholar
[4]	龚少康, 周静, 王志青, 朱茂聪, 沈杰, 吴智, 陈文 2021 物理学报 70 197301 Google Scholar Gong S K, Zhou J, Wang Z Q, Zhu M C, Shen J, Wu Z, Chen W 2021 Acta Phys. Sin. 70 197301 Google Scholar
[5]	Guo T T, Huang H X, Huang X L, Wang Y, Duan L, Xu Z 2022 J. Alloys Compd. 921 166218 Google Scholar
[6]	More K D, Narwade V N, Halge D I, Dadge J W, Bogle K A 2020 Physica B 595 412339 Google Scholar
[7]	He H K, Yang R, Zhou W, Huang H M, Xiong J, Gan L, Zhai T Y, Guo X 2018 Small 14 1800079 Google Scholar
[8]	Zhou H, Wei X D, Wei W, Ye C, Zhang R L, Zhang L, Xia Q, Huang H, Wang B 2019 Surf. Coat. Tech. 359 150 Google Scholar
[9]	张娇娇, 周龙, 王洪强, 董广志, 樊慧庆 2023 铸造技术 44 23 Google Scholar Zhang J J, Zhou L, Wang H Q, Dong G Z, Fan H Q 2023 Foundry Technology 44 23 Google Scholar
[10]	Wang Y H, He Z Q, Lai X B, Liu B Y, Chen Y B, Zhang L W, Wang F P 2021 J. Alloys Compd. 873 159809 Google Scholar
[11]	Strukov D B, Snider G S, Stewart D R, Williams R S 2008 Nature 453 80 Google Scholar
[12]	Zhang L, Huang H, Ye C, Chang K C, Zhang R L, Xia Q, Wei X D, Wei W, Wang W F 2018 Semicond. Sci. Tech. 33 085013 Google Scholar
[13]	代月花, 潘志勇, 陈真, 王菲菲, 李宁, 金波, 李晓风 2016 物理学报 65 073101 Google Scholar Dai Y H, Pan Z Y, Chen Z, Wang F F, Li N, Jin B, Li X F 2016 Acta Phys. Sin. 65 073101 Google Scholar
[14]	Leydecker T, Herder M, Pavlica E, Bratina G, Hecht S, Orgiu E, Samorì P 2016 Nat Nanotechnol. 11 769 Google Scholar
[15]	Lee Y J, Liu K H, Peng Y, Yen M C, Tamada K 2020 Nat. Commun. 12 4460 Google Scholar
[16]	曾凡菊, 谭永前, 唐孝生, 张小梅, 尹海峰 2021 物理学报 70 157301 Google Scholar Zeng F J, Tan Y Q, Tang X S, Zhang X M, Yin H F 2021 Acta Phys. Sin. 70 157301 Google Scholar
[17]	Ge N N, Gong C H, Yuan X C, Zeng H Z, Wei X H 2018 RSC Adv. 8 29499 Google Scholar
[18]	Kao M C, Chen H Z, Chen K H, Shi J B, Chen K P 2020 Thin Solid Films 697 137816 Google Scholar
[19]	Chen Z L, Yu Y, Jin L F, Li Y F, Li Q Y, Li T T, Li J, Zhao H L, Zhang Y T, Dai H T 2021 J. Mater Chem. C 8 2178 Google Scholar
[20]	Singh L, Kaushik V, Rajput S, Kumar M 2021 J. Lightwave Technol. 39 5869 Google Scholar
[21]	Ungureanu M, Zazpe R, Golmar F, Stoliar P, Llopis R, Casanova F, Hueso L E 2012 Adv. Mater. 24 2496 Google Scholar
[22]	Zhu X J, Lu W D 2018 Acs Nano 12 1242 Google Scholar
[23]	Russo P, Xiao M, Liang R, Zhou N Y 2018 Adv Funct. Mater. 28 17062301 Google Scholar
[24]	Xie S, Pei L, Li M Y, Zhu Y D, Cheng X Y, Ding H Q, Xiong R 2018 J. Alloys Compd. 778 141 Google Scholar
[25]	Xue W H, Ci W J, Xu X H, Liu G 2020 Chin. Phys. B. 29 048401 Google Scholar
[26]	Sharath S U, Bertaud T, Kurian J, Hildebrandt E, Walczyk C, Calka P, Zaumseil P, Sowinska M, Walczyk D, Gloskovskii A, Schroeder T, Alff L 2014 Appl. Phys. Lett. 104 063502 Google Scholar
[27]	Guo T T, Wang Y X, Duan L, Fan J B, Wang Z Z 2021 Vacuum 189 110224 Google Scholar
[28]	Bon C Y, Kim D, Lee K, Choi S, Yoo S I 2020 AIP Adv. 10 115117 Google Scholar
[29]	Kannadasan N, Shanmugam N, Cholan S, Sathishkumar K, Viruthagiri G, Poonguzhali R 2014 Current Appl. Phys. 14 1760 Google Scholar
[30]	Pereira L, Barquinha P, Fortunato E, Martins R 2005 Mater. Sci Engineer B 118 210 Google Scholar
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[32]	Wu P, Zhang J, Lu J G, Li X F, Wu C J, Sun R J, Feng L S, Jiang Q J, Lu B, Pan X H 2014 IEEE T Electron. Dev. 61 1431 Google Scholar
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[34]	Laiho R, Poloskin D S, Stepanov Y P, Vlasenko M P, Vlasenko L S, Zakhvalinskii V S 2009 J Appl. Phys. 106 56 Google Scholar
[35]	Wang X J, Wang Y Y, Feng M, Wang K Y, Tian Y M 2020 Current Appl. Phys. 20 261104 Google Scholar
[36]	Tan T T, Du Y H, Sun Y L, Zhang H, Cao A, Zha G Q 2019 J. Mater. Sci. 30 13445 Google Scholar

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光电协同调控下HfO_x基阻变存储器的阻变特性