Effects of electrode materials and bias polarities on breakdown behaviors of oxide dielectrics and their mechanisms

Wang Yan-Bin; Liu Qian; Wang Yong; Dai Bo; Wei Xian-Hua

doi:10.7498/aps.70.20201262

Abstract

The memristors and the energy storage capacitors have the same sandwich structure, but the operating voltages required by the two devices are significantly different. Therefore, in the same device, it is necessary to study the influencing factors of operating voltage and adjust the operating voltage of the devices to realize the applications of the device in diverse fields. The polycrystalline ZrO₂ and amorphous TaO_x thin films are deposited on ITO conductive glass and Pt/Si substrates by reactive magnetron sputtering technology. Au, Ag and Al metal materials are selected as the top electrodes to construct a variety of metal/insulator/metal sandwich capacitors. The breakdown strengths of these devices under different bias polarities are studied. The results demonstrate that the breakdown strength is slightly larger for the ZrO₂ based capacitor with ITO as the bottom electrode than for the Pt electrode device under negative bias. The breakdown electric field of the device with Ag as the top electrode shows obvious dependence on bias polarity, no matter whether the bottom electrode is ITO or Pt. The breakdown strength is reduced by more than an order of magnitude under a positive bias (2.13 MV/cm) compared with under a negative bias (0.17 MV/cm) of Ag/ZrO₂/ITO device. The breakdown strength of the Al/TaO_x/Pt device is enhanced under the forward bias (3.6 MV/cm), contrary to the Ag electrode device, which is nearly twice higher than the breakdown electric field under the negative bias (1.81 MV/cm). The different breakdown behaviors of the above devices can be explained by the migration and rearrangement of oxygen between the oxide electrode and the dielectric interface layer; the dissolution, migration and reduction of the electrochemically active metal electrode; and the redox reaction between the chemically active metal electrode and the oxide dielectric interface. The ZrO₂ based capacitor with ITO electrode undergoes a redox reaction of Sn⁴⁺ in the ITO under negative bias, forming an insulating layer at the interface between the dielectric layer and the ITO electrode, which contributes a larger breakdown electric field. In addition, the electrochemical metallization process happens to the Ag electrode device under positive bias, and the breakdown electric field is smaller than negative bias due to the large diffusion coefficient of Ag ions in the film, while breakdown is dominated by the defect characteristics of the dielectric film under negative bias. The Al/TaO_x/Pt devices can form AlO_x oxide layer under positive bias, spontaneously, which can inhibit the leakage current, and also act as a series resistance to disperse part of the voltage and enhance the breakdown voltage of the device. The experimental results have guided significance in designing and operating the devices with different operating voltage requirements, such as memristors and dielectric energy storage capacitors.

Keywords:

Authors and contacts

State Key Laboratory of Environment-friendly Energy Materials, Southwest University of Science and Technology, Mianyang 621010, China

Corresponding author: Wei Xian-Hua, weixianhua@swust.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51772252), the Science and Technology Program of Sichuan Province, China (Grant No. 2020JDRC0062), and the State Key Laboratory of Environment-friendly Energy Materials Program, Southwest University of Science and Technology, Mianyang, China (Grant Nos. 18FKSY0202, 19FKSY09)

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References

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Cited By

图 1 MIM器件用于阻变及储能电容器时的机理图以及对工作电压的要求

Figure 1. Schematic diagram of the MIM devices for resistive switching and energy storage with different operation voltages.

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图 2 ZrO₂和TaO_x薄膜的XRD, AFM和SEM图　(a) ITO基底上沉积的ZrO₂薄膜; (b) Pt/Si基底上沉积的ZrO₂薄膜; (c) Pt/Si 基底上沉积的TaO_x薄膜

Figure 2. XRD, AFM and SEM patterns of the ZrO₂ and TaO_x thin films: (a) The ZrO₂ thin film deposited on ITO/glass; (b) the ZrO₂ thin film deposited on Pt/Si; (c) the TaO_x thin film deposited on Pt/Si.

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图 3 ZrO₂基电容器的I-E特征曲线　(a) Ag/ZrO₂/Pt和Au/ZrO₂/Pt器件; (b) Ag/ZrO₂/ITO和Au/ZrO₂/ITO器件

Figure 3. I-E characteristics of ZrO₂ based capacitors: (a) Ag/ZrO₂/Pt and Au/ZrO₂/Pt; (b) Ag/ZrO₂/ITO and Au/ZrO₂/ITO.

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图 4 ZrO₂基电容器在正负偏压下的击穿电场统计图

Figure 4. Statistical charts of positive and negative breakdown electric field of ZrO₂-based capacitors.

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图 5 Pt/Si基底上TaO_x基器件　(a) I-E特征曲线; (b)正负偏压下击穿电场值统计图

Figure 5. Positive and negative breakdown electric field of TaO_x based devices: (a) I-E characteristics; (b) statistical charts.

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图 6 器件在施加偏压下的击穿机理示意图　(a)负偏压下的Au/ZrO₂/ITO器件; (b), (c) 正负偏压下的Ag/ZrO₂/Pt器件; (d) 正偏压下的Al/TaO_x/Pt器件

Figure 6. Schematic diagrams of the breakdown mechanisms of the devices under different applied biases: (a) The Au/ZrO₂/ITO device under negative bias; (b), (c) Ag/ZrO₂/Pt devices under positive and negative biases, respectively; (d) the Al/TaO_x/Pt device under positive bias.

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map

[1]	Chua L 1971 IEEE Trans. Circuit Theory 18 507 Google Scholar
[2]	Hao X 2013 J. Adv. Dielectr. 3 1330001 Google Scholar
[3]	Palneedi H, Peddigari M, Hwang G T, Jeong D Y, Ryu J 2018 Adv. Funct. Mater. 28 1803665 Google Scholar
[4]	Zheng T, Wu J, Xiao D, Zhu J 2018 Prog. Mater Sci. 98 552 Google Scholar
[5]	Wang Y, Jie W, Yang C, Wei X, Hao J 2019 Adv. Funct. Mater. 29 1808118 Google Scholar
[6]	Wang Y, Hu L, Wei X, Zhuge F 2020 Appl. Phys. Lett. 116 221602 Google Scholar
[7]	Choi J, Park S, Lee J, Hong K, Kim D H, Moon C W, Park G D, Suh J, Hwang J, Kim S Y, Jung H S, Park N G, Han S, Nam K T, Jang H W 2016 Adv. Mater. 28 6562 Google Scholar
[8]	Hu L, Fu S, Chen Y, Cao H, Liang L, Zhang H, Gao J, Wang J, Zhuge F 2017 Adv. Mater. 29 1606927 Google Scholar
[9]	Guo J, Wang L, Liu Y, Zhao Z, Zhu E, Lin Z, Wang P, Jia C, Yang S, Lee S J, Huang W, Huang Y, Duan X 2020 Matter 2 965 Google Scholar
[10]	Guo X, Wang Q, Lü X, Yang H, Sun K, Yang D, Zhang H, Hasegawa T, He D 2020 Nanoscale 12 4320 Google Scholar
[11]	Liu Y, Ye C, Chang K C, Li L, Jiang B, Xia C, Liu L, Zhang X, Liu X, Xia T, Peng Z, Cao G, Cheng G, Ke S, Wang J 2020 Small 16 2004619 Google Scholar
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[13]	Yang L, Kong X, Li F, Hao H, Cheng Z, Liu H, Li J F, Zhang S 2019 Prog. Mater Sci. 102 72 Google Scholar
[14]	Pan F, Gao S, Chen C, Song C, Zeng F 2014 Mater. Sci. Eng. R. 83 1 Google Scholar
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[16]	Liu Q, Sun J, Lü H, Long S, Yin K, Wan N, Li Y, Sun L, Liu M 2012 Adv. Mater. 24 1844 Google Scholar
[17]	Liu S, Lu N, Zhao X, Xu H, Banerjee W, Lü H, Long S, Li Q, Liu Q, Liu M 2016 Adv. Mater. 28 10623 Google Scholar
[18]	Li Q, Qiu L, Wei X, Dai B, Zeng H 2016 Sci. Rep. 6 29347 Google Scholar
[19]	Tian B, Nukala P, Hassine M B, Zhao X, Wang X, Shen H, Wang J, Sun S, Lin T, Sun J, Ge J, Huang R, Duan C, Reiss T, Varela M, Dkhil B, Meng X, Chu J 2017 Phys. Chem. Chem. Phys. 19 16960 Google Scholar
[20]	Gao W, Yao M, Yao X 2017 Ceram. Int. 43 13069 Google Scholar
[21]	Gao W, Yao M, Yao X 2018 ACS Appl. Mater. Interfaces 10 28745 Google Scholar
[22]	Hou C, Huang W, Zhao W, Zhang D, Yin Y, Li X 2017 ACS Appl. Mater. Interfaces 9 20484 Google Scholar
[23]	Panda D, Tseng T Y 2013 Thin Solid Films 531 1 Google Scholar
[24]	Kudoh Y, Akami K, Matsuya Y 1999 Synth. Met. 102 973 Google Scholar
[25]	Matsuhashi H, Nishikawa S 1994 Jpn. J. Appl. Phys. 33 1293 Google Scholar
[26]	Atanassova E, Paskaleva A 2007 Microelectron. Reliab. 47 913 Google Scholar
[27]	Lee M J, Lee C B, Lee D, Lee S R, Chang M, Hur J H, Kim Y B, Kim C J, Seo D H, Seo S, Chung U I, Yoo I K, Kim K 2011 Nat. Mater. 10 625 Google Scholar
[28]	Wu M C, Wu T H, Tseng T Y 2012 J. Appl. Phys. 111 014505 Google Scholar
[29]	Liu Q, Long S, Wang W, Tanachutiwat S, Li Y, Wang Q, Zhang M, Huo Z, Chen J, Liu M 2010 IEEE Electron Device Lett. 31 1299 Google Scholar
[30]	Li Y, Long S, Zhang M, Liu Q, Shao L, Zhang S, Wang Y, Zuo Q, Liu S, Liu M 2009 IEEE Electron Device Lett. 31 117 Google Scholar
[31]	Li C, Wang F, Zhang J, She Y, Zhang Z, Liu L, Liu Q, Hao Y, Zhang K 2020 ECS J. Solid State Sci. Technol 9 041005 Google Scholar
[32]	Atanassova E, Spassov D, Paskaleva A 2006 Microelectron. Eng. 83 1918 Google Scholar
[33]	Kindsmüller A, Meledin A, Mayer J, Waser R, Wouters D J 2019 Nanoscale 11 18201 Google Scholar
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[35]	Ye C, Zhan C, Tsai T M, Chang K C, Chen M C, Chang T C, Deng T, Wang H 2014 Appl. Phys. Express 7 034101 Google Scholar
[36]	Zhang J, Wang F, Li C, Shan X, Liang A, Hu K, Li Y, Liu Q, Hao Y, Zhang K 2020 Appl. Surf. Sci. 526 146723 Google Scholar
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