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摘要

忆阻器和能量存储电容器具有相同的三明治结构, 然而两个器件需要的操作电压有明显差异, 因此在同一个器件中, 研究操作电压的影响因素并对操作电压进行调控, 实现器件在不同领域的应用是十分必要的一个工作. 本文利用反应磁控溅射技术在ITO导电玻璃、Pt/Si基底上生长了多晶ZrO ₂和非晶TaO _x薄膜, 选用不同金属材料Au, Ag和Al用作上电极构建了多种金属/氧化物介质/金属三明治结构的电容器, 研究了器件在不同偏压极性下的击穿强度. 结果发现: 底电极是ITO的ZrO ₂基电容器在负偏压下的击穿电场比Pt电极器件稍大. 不管底电极是ITO还是Pt, Ag作为上电极时器件的击穿强度均存在明显的偏压极性依赖性, 正偏压下的击穿电场减小了一个数量级; 相反, 在Al作为上电极的Al/TaO _x/Pt器件中, 正向偏压比负向偏压下的击穿电场增加了近2倍. 上述器件的不同击穿行为分别可以由氧化物电极和介质界面层间氧的迁移和重排、电化学活性金属电极的溶解迁移和还原以及化学活性金属电极与氧化物界面的氧化还原反应来解释. 该实验结果对有不同操作电压要求的器件, 如忆阻器和介质储能电容器等在器件设计和操作方面具有指导意义.

关键词:

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 ZrO ₂and amorphous TaO _xthin 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 ZrO ₂based 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/ZrO ₂/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 ZrO ₂based capacitor with ITO electrode undergoes a redox reaction of Sn ⁴⁺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 _xoxide 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:

作者及机构信息

通信作者:魏贤华,weixianhua@swust.edu.cn

基金项目:国家自然科学基金(批准号: 51772252)、四川省科技计划(批准号: 2020JDRC0062)和西南科技大学环境友好能源材料国家重点实验室项目(批准号: 18FKSY0202, 19FKSY09)资助的课题

Authors and contacts

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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施引文献

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