Size-controlled resistive switching performance and regulation mechanism of SnO<sub>2</sub> QDs

Gong Shao-Kang; Zhou Jing; Wang Zhi-Qing; Zhu Mao-Cong; Shen Jie; Wu Zhi; Chen Wen

doi:10.7498/aps.70.20210608

Abstract

As a non-volatile memory, zero-dimensional quantum dot resistive random access memory (RRAM) has shown broad application prospects in the field of intelligent electronic devices due to its advantages of simple structure, low switching voltage, fast response speed, high storage density, and low power consumption. Tin dioxide quantum dots (SnO₂ QDs) are a good option for resistive functional materials with excellent physical and chemical stabilities, high electron mobilities, and adjustable energy band structures. In this paper, the SnO₂ QDs with sizes of 2.51 nm, 2.96 nm and 3.53 nm are prepared by the solvothermal method, and the quantum size effect is observed in a small size range and the effective regulation of resistive switching voltage is achieved based on its quantum size effect, which is the unique advantage of quantum dot material in comparison with that of bulk material. Research result shows that as the size of SnO₂ QD increases, the SET/RESET voltage gradually decreases from –3.18 V/4.35 V to –2.02 V/3.08 V. The 3.53 nm SnO₂ QDs have lower SET/RESET voltage (–2.02 V/3.08 V) and larger resistive switching ratio (> 10⁴), and the resistive switching performance of the device has changed less than 5% after having experienced durability tests 2 × 10⁴ times, showing good stability and retention. Besides, according to the fitting of charge transport mechanism, SnO₂ QD RRAM exhibits Ohmic conduction under LRS, while Ohmic conduction, thermionic emission and space charge limit current work together during HRS. The resistive switching effect of SnO₂ QDs is controlled by trap filled limit current and interface Schottky Barrier modulation; the trapping/de-trapping behavior of internal defect potential well of SnO₂ QDs on electrons dominates the HRS/LRS switching, while the effective control of ITO/SnO₂ QDs and SnO₂ QDs/Au interface Schottky barrier is the key to accurately regulating the switching voltage. The reason why SnO₂ QD RRAM exhibits good size-switching voltage dependence is that the larger SnO₂ QD has lower Fermi level and interface Schottky barrier height, so the junction resistance voltage division is reduced, and the SET/RESET voltage decrease accordingly. This work reveals the huge application potential and commercial application value of SnO₂ QDs in the field of resistive switching memory, and provides a new option for the development of RRAM.

Keywords:

Authors and contacts

1.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China
2.
School of Materials and Chemistry Engineering, Hunan Institute Technology, Hengyang 421002, China

Corresponding author: Zhou Jing, zhoujing@whut.edu.cn

Funds: Project Supported by the National Natural Science Foundation of China (Grant Nos. 51572205, 51802093), the National Key R&D Program of China (Grant No. 2016YFB0303904), the Fundamental Research Fund for the Central Universities, China (Grant Nos. WUT: 2018III019, 2019IVA108, 2020III021), and the Scientific Research Project of Hunan Education Department, China (Grant No. 20B161)

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References

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Cited By

图 1 不同反应温度下制备的SnO₂ QDs 的TEM图像　(a) 160 ℃; (b) 180 ℃; (c) 200 ℃. 插图分别为对应的SnO₂ QDs尺寸分布直方图. 3.53 nm SnO₂ QDs的(d)局部HRTEM图像, (e) 选区电子衍射图像与(f) EDS能谱分析

Figure 1. TEM images of SnO₂ QDs prepared at (a) 160 ℃, (b) 180 ℃ and (c) 200 ℃. Inset gives the distribution histogram of SnO₂ QDs size. (d) Magnified TEM image, (e) SAED pattern and (f) EDS spectrum of 3.53 nm SnO₂ QDs.

DownLoad: Full-Size Img PowerPoint

图 2 SnO₂ QDs的UPS图谱　(a) 2.51 nm; (b) 2.96 nm; (c) 3.53 nm. 插图为费米边、二次电子截止边截距. 不同尺寸SnO₂ QDs 的(d) UV-vis光谱, (e) 光学禁带曲线及(f) 能带结构示意图

Figure 2. UPS spectra of (a) 2.51 nm, (b) 2.96 nm and (c) 3.53 nm of SnO₂ QDs, and insets shows the Secondary electron cutoff and Fermi edge intercepts. (d) UV-vis absorption spectra, (e) optical band gaps plots and (f) energy band structure of SnO₂ QDs with different sizes.

DownLoad: Full-Size Img PowerPoint

图 3 (a) ITO与(b) SnO₂ QDs薄膜的表面SEM图像. (c) SnO₂ QDs RRAM的器件结构示意图及(d) 横截面FESEM图像

Figure 3. Surface SEM picture of (a) ITO and (b) SnO₂ QDs film. (c) Device structure schematic diagram of SnO₂ QDs RRAM and its (d) cross-sectional FESEM image.

DownLoad: Full-Size Img PowerPoint

图 4 (a) 不同尺寸下SnO₂ QDs RRAM的I-V特性曲线; (b) SET/RESET电压随SnO₂ QDs尺寸的变化曲线; (c) 不同尺寸SnO₂ QDs RRAM的循环稳定性曲线, 插图为施加的脉冲电压直方图; (d) 3.53 nm SnO₂ QDs RRAM的SET/RESET电压频率分布直方图

Figure 4. (a) I-V curves of SnO₂ QDs RRAM with different sizes; (b) variation of SET/RESET voltage with SnO₂ QDs size; (c) cycle stability tests of SnO₂ QDs RRAM and inset shows the impulse voltage curve; (d) SET/RESET voltage distribution of 3.53 nm SnO₂ QDs RRAM.

DownLoad: Full-Size Img PowerPoint

图 5 3.53 nm SnO₂ QDs RRAM在(a) SET过程, (b) RESET过程的电导机制拟合曲线; 局部区域的电导机制拟合(c) SET过程V₁-V_SET阶段, (d) RESET过程V₂-V_max阶段

Figure 5. Conduction mechanism fitting curves of (a) SET process and (b) RESET process on 3.53 nm SnO₂ QDs RRAM. Local region of conduction mechanism (c) stage of V₁-V_SET in SET process; (d) stage of V₂-V_max in RESET process.

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图 6 (a) ITO/SnO₂ QDs/Au界面势垒模型; 各阶段的阻变行为 (b) 热电子发射区域; (c) SET过程; (d) RESET过程; (e) SCLC区域; (f) RESET阶段热电子发射区域

Figure 6. (a) Schematic diagram of ITO/SnO₂ QDs/Au interfacial barrier model and resistive switching behavior in (b) thermionic emission, (c) SET, (d) RESET, (e) SCLC, (f) thermionic emission of RESET process.

DownLoad: Full-Size Img PowerPoint

[1]	Chen A 2016 Solid-State Electron. 125 25 Google Scholar
[2]	Chang T C, Chang K C, Tsai T M, Chu T J, Sze S M 2016 Mater. Today 19 254 Google Scholar
[3]	Li Y, Chu J, Duan W, Cai G, Fan X, Wang X, Wang G, Pei Y 2018 ACS Appl. Mater. Interfaces 10 24598 Google Scholar
[4]	史晨阳, 闵光宗, 刘向阳 2020 物理学报 69 178702 Google Scholar Shi C Y, Min G Z, Liu X Y 2020 Acta Phys. Sin. 69 178702 Google Scholar
[5]	Zhou G, Yang X, Xiao L, Sun B, Zhou A 2019 Appl. Phys. Lett. 114 163506 Google Scholar
[6]	Gao S, Yi X, Shang J, Liu G, Li R W 2019 Chem. Soc. Rev. 48 1531 Google Scholar
[7]	Zhou D, Chen F G, Han S, Hu W, Zang Z G, Hu Z P, Li S Q, Tang X S 2018 Ceram. Int. 44 S152 Google Scholar
[8]	孙劲鹏, 王太宏 2003 物理学报 52 2563 Google Scholar Sun J P, Wang T H 2003 Acta Phys. Sin 52 2563 Google Scholar
[9]	Datta S 2013 Quantum Transport: Atom to Transistor (England: Cambridge University Press) pp18, 170, 285
[10]	Fan F, Zhang B, Cao Y, Yang X, Gu J, Chen Y 2017 Nanoscale 9 10610 Google Scholar
[11]	Yan X, Pei Y, Chen H, Zhao J, Zhou Z, Wang H, Zhang L, Wang J, Li X, Qin C, Wang G, Xiao Z, Zhao Q, Wang K, Li H, Ren D, Liu Q, Zhou H, Chen J, Zhou P 2019 Adv. Mater. 31 1805284 Google Scholar
[12]	Younis A, Chu D, Mihail I, Li S 2013 ACS Appl. Mater. Interfaces 5 9429 Google Scholar
[13]	Wang Z Q, Liu Y L, Shen J, Chen W, Miao J, Li A, Liu K, Zhou J 2020 Sci. China Mater. 63 2497 Google Scholar
[14]	Chen Z, Zhang Y, Yu Y, Cao M, Che Y, Jin L, Li Y, Li Q, Li T, Dai H, Yang J, Yao J 2019 Appl. Phys. Lett. 114 181103 Google Scholar
[15]	Wang H, Yan X B 2019 Phys. Status Solidi RRL 13 1900073 Google Scholar
[16]	Banerjee W, Liu Q, Long S B, Lv H B, Liu M 2017 J. Phys. D: Appl. Phys. 50 303002 Google Scholar
[17]	Hwang B H, Lee J S 2018 Adv. Electron. Mater. 5 1800519
[18]	贾林楠, 黄安平, 郑晓虎, 肖志松, 王玫 2012 物理学报 61 217306 Google Scholar Jia L N, Huang A P, Zheng X H, Xiao Z S, Wang M 2012 Acta Phys. Sin. 61 217306 Google Scholar
[19]	Chen K Q, Zhou J, Chen W, Zhou P, He F, Liu Y L 2015 Part. Part. Syst. Char. 32 999 Google Scholar
[20]	Chen D Y, Huang S H, Huang R, Zhang Q, Le T T, Cheng E, Hu Z J, Chen Z W 2018 Mater. Res. Lett. 6 462 Google Scholar
[21]	Xu Z M, Guan P Y, Younis A, Chu D W, Li S 2017 RSC Adv. 7 56390 Google Scholar
[22]	Sarkar P K, Bhattacharjee S, Prajapat M, Roy A 2015 RSC Adv. 5 105661 Google Scholar
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[24]	Onlaor K, Thiwawong T, Tunhoo B 2014 Org. Electron. 15 1254 Google Scholar
[25]	Braun D 2010 J. Polym. Sci. Pol. Phys. 41 2622
[26]	Zhang X G, Pantelides S T 2012 Phys. Rev. Lett. 108 266602 Google Scholar
[27]	Valov I, Waser R, Jameson J R, Kozicki M N 2011 Nanotechnology 22 254003 Google Scholar
[28]	Waser R, Dittmann R, Staikov G, Szot K 2009 Adv. Mater. 21 2632 Google Scholar
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[30]	Zhang P, Xu B, Gao C, Chen G L, Gao M Z 2016 ACS Appl. Mater. Interfaces 8 30336 Google Scholar
[31]	Nieh C H, Lu M L, Weng T M, Chen Y F 2014 Appl. Phys. Lett. 104 1951
[32]	刘东青, 程海峰, 朱玄, 王楠楠, 张朝阳 2014 物理学报 63 187301 Google Scholar Liu D Q, Cheng H F, Zhu X, Wang N N, Zhang C Y 2014 Acta Phys. Sin. 63 187301 Google Scholar
[33]	Dash C S, Prabaharan S R S 2019 Rev. Adv. Mater. Sci. 58 248 Google Scholar
[34]	Jeong J S, Topsakal M, Xu P, Jalan B, Wentzcovitch R M, Mkhoyan K A 2016 Nano Lett. 16 6816 Google Scholar
[35]	Kumar A, Mukherjee S, Kranti A 2018 J. Phys. D: Appl. Phys. 51 405601 Google Scholar
[36]	Hsu C C, Wang S Y, Lin Y S, Chen Y T 2018 J. Alloys Compd. 779 609
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[40]	Liu Y, Guo J, Zhu E B, Liao L, Lee S J, Ding M N, Shakir I, Gambin V, Huang Y, Duan X F 2018 Nature 557 696 Google Scholar

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Size-controlled resistive switching performance and regulation mechanism of SnO₂ QDs

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Corresponding author: Zhou Jing, zhoujing@whut.edu.cn

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Size-controlled resistive switching performance and regulation mechanism of SnO2 QDs

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Corresponding author: Zhou Jing, zhoujing@whut.edu.cn

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Size-controlled resistive switching performance and regulation mechanism of SnO₂ QDs