Resistive properties of CuInS<sub>2</sub> quantum dots regulated by niobium-doped lead zirconate titanate ferroelectric films

Zhu Mao-Cong; Shao Ya-Jie; Zhou Jing; Chen Wen; Wang Zhi-Qing; Tian Jing

doi:10.7498/aps.71.20220911

Abstract

As a new type of non-volatile memory, quantum dot resistive random access memory (RRAM) has attracted much attention for its easy preparation, fast responding time, high storage density, and smaller device size. CuInS₂ quantum dot (CuInS₂ QD) is a kind of excellent resistive functional material with abundant electron capture sites, high optical absorption coefficient, and high carrier mobility. In this work, CuInS₂ QDs/Nb:Pb (Zr_0.52Ti_0.48)O₃ (PNZT) films are prepared by spin-coating CuInS₂ QDs on PNZT films. The results show that the resistive properties of CuInS₂ QDs RRAMs can be effectively improved by introducing PNZT films and can be controlled by changing the polarization direction. The CuInS₂ QDs/PNZT film in the negative polarization state promotes the interfacial electrons to enter into the PNZT film, which will reduce the height of the interfacial barrier and the thickness of the interfacial depletion region. And it will reduce the resistance of the composite film at the low resistance state (LRS). Compared with the switching voltage and resistive switching ratio of the pure CuInS₂ QDs film (10³), the switching voltage of the device decreases to –4.1/3.4 V and the resistive switching ratio increases to 10⁶. Furthermore, it maintains good stability in the 10³ cycle durability test. In contrast, the CuInS₂ QDs/PNZT film interface has a larger barrier height and depletion-layer thickness when the PNZT is in the positive polarization state, which increases the resistance of the composite film in the LRS state. As a result, the switching voltage of the device increases to –6.4/5.7 V with a resistive switching ratio of 10⁴. The resistive properties of the CuInS₂ QDs/PNZT film can be tuned by changing the polarization direction, as the polarization direction of the PNZT changes the interfacial energy band structure and affects the conduction mechanism. This work reveals the feasibility of using ferroelectric thin films to improve the resistive properties of quantum dots RRAMs and thus providing an approach to further developing RRAMs.

Keywords:

Authors and contacts

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

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

Funds: Project supported by the Key Research and Development Project of Hubei Province, China (Grant No. 2021BAA214) and the Sanya Science and Education Innovation Park of Wuhan University of Technology, China (Grant Nos. 2020KF0026, 2021KF0013).

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References

[1]	Wang Z J, Bai Y 2019 Small 15 1805088 Google Scholar
[2]	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
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[7]	Wang Y, Lü Z, Chen J, Wang Z, Zhou Y, Zhou L, Chen X, Han S T 2018 Adv. Mater. 30 1802883 Google Scholar
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[9]	Chen Z, He L, Zhang F, Jiang J, Meng J, Zhao B, Jiang A 2013 J. Appl. Phys. 113 184106 Google Scholar
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图 1 CuInS₂ QDs/PNZT RRAM结构示意图

Figure 1. Schematic diagram of CuInS₂ QDs/PNZT RRAM structure.

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图 2 (a) CuInS₂ QDs的TEM图像 (插图为CuInS₂ QDs 尺寸分布直方图); (b) CuInS₂ QDs的HRTEM图像; (c) CuInS₂ QDs的XRD图谱

Figure 2. (a) TEM image of CuInS₂ QDs (Inset is the size distribution histogram of CuInS₂ QDs); (b) HRTEM image of CuInS₂ QDs; (c) XRD pattern of CuInS₂ QDs.

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图 3 PNZT薄膜的XRD图谱 (a) 和电滞回线 (b)

Figure 3. XRD pattern (a) and hysteresis loop (b) of PNZT film.

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图 4 (a) CuInS₂ QDs/PNZT RRAM的断面FESEM图像; (b) PNZT薄膜与(c) CuInS₂ QDs薄膜的表面FESEM图像; (d) CuInS₂ QDs薄膜表面元素分布图

Figure 4. (a) Cross-sectional FESEM image of CuInS₂ QDs/PNZT RRAM; FESEM image of the surface for (b) PNZT film and (c) CuInS₂ QDs film; (d) surface element distribution of CuInS₂ QDs film.

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图 5 CuInS₂ QDs RRAM与正负向和无极化下CuInS₂ QDs/PNZT RRAM的 (a) I-V曲线与 (b) 开关电压直方图; (c) CuInS₂ QDs RRAM循环稳定性测试; (d) 无极化, (e) 负向极化和 (f) 正向极化的CuInS₂ QDs/PNZT RRAM循环稳定性测试(插图为施加的脉冲电压)

Figure 5. (a) I-V curves and (b) SET/RESET voltage histograms of CuInS₂ QDs RRAM and CuInS₂ QDs/PNZT RRAM with the different polarization orientations; (c) cycling stability test of CuInS₂ QDs RRAM; cycling stability test of (d) no polarized, (e) negative polarized and (f) positive polarized CuInS₂ QDs/PNZT RRAM (Inset is the applied pulse voltage).

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图 6 CuInS₂ QDs RRAM在(a) 设置过程及(b) 复位过程的拟合曲线

Figure 6. Fitting curves of CuInS₂ QDs RRAM during (a) set process and (b) reset process.

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图 7 负向极化下CuInS₂ QDs/PNZT RRAM (a) 设置过程及(b) Slope10阶段的拟合曲线, (c) 复位过程及(d) Slope15阶段的拟合曲线; 正向极化下CuInS₂ QDs/PNZT RRAM (e) 设置过程及(f) Slope18阶段的拟合曲线, (g) 复位过程及(h) Slope23阶段的拟合曲线

Figure 7. Fitting curves of CuInS₂ QDs/PNZT RRAM under negative polarization in (a) set process and (b) Slope10 stage, (c) reset process and (d) Slope15 stage; fitting curves of CuInS₂ QDs/PNZT RRAM under positive polarization in (e) set process and (f) Slope18 stage, (g) reset process and (h) Slope23 stage.

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图 8 PNZT薄膜的光学性能　(a) UV-Vis光谱图; (b) 光学带隙图; (c) PNZT薄膜的UPS; (d) 二次电子截止边谱和费米边谱

Figure 8. Optical performance of PNZT films: (a) UV-Vis spectrum; (b) optical band gap; (c) UPS of PNZT film; (d) secondary electron cutoff and Fermi edge intercepts.

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图 9 (a) PNZT与CuInS₂ QDs的能带结构. CuInS₂ QDs/PNZT复合薄膜界面能带结构示意图　(b) 无极化; (c) 负向极化; (d) 正向极化

Figure 9. (a) Band structures of PNZT and CuInS₂ QDs. Schematic diagram of the interfacial band structure of CuInS₂ QDs/PNZT film: (b) No polarization; (c) negative polarization; (d) positive polarization.

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表 1 不同器件的阻变性能

Table 1. Resistance switching performance of the different devices.

测试单元	工作电压/V	阻变开关比
CuInS₂ QDs RRAM	–4.5/4.5	3.4×10³
无极化PNZT/CuInS₂ QDs RRAM	–5.6/5.0	1.7×10⁵
正向极化PNZT/CuInS₂ QDs RRAM	–6.4/5.7	1.8×10⁴
负向极化PNZT/CuInS₂ QDs RRAM	–4.1/3.4	4.8×10⁶

DownLoad: CSV

[1]	Wang Z J, Bai Y 2019 Small 15 1805088 Google Scholar
[2]	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
[3]	Lü Z Y, Wang Y, Chen J G, Wang J J, Zhou Y, Han S T 2020 Chem. Rev. 120 3941 Google Scholar
[4]	Yan X B, Pei Y F, Chen H W, et al. 2019 Adv. Mater. 31 1805284 Google Scholar
[5]	Han S T, Hu L, Wang X, Zhou Y, Zeng Y J, Ruan S, Pan C, Peng Z 2017 Adv. Sci. 4 1600435 Google Scholar
[6]	Kim T W, Yang Y, Li F, Kwan W L 2012 NPG Asia Mater. 4 e18 Google Scholar
[7]	Wang Y, Lü Z, Chen J, Wang Z, Zhou Y, Zhou L, Chen X, Han S T 2018 Adv. Mater. 30 1802883 Google Scholar
[8]	Thomas A, Resmi A, Ganguly A, Jinesh K 2020 Sci. Rep. 10 12450 Google Scholar
[9]	Chen Z, He L, Zhang F, Jiang J, Meng J, Zhao B, Jiang A 2013 J. Appl. Phys. 113 184106 Google Scholar
[10]	贾林楠, 黄安平, 郑晓虎, 肖志松, 王玫 2012 物理学报 21 217306 Google Scholar Jia L N, Huang A P, Zheng X H, Xiao Z S, Wang Z 2012 Acta Phys. Sin. 21 217306 Google Scholar
[11]	Fan Z, Fan H, Yang L, Li P, Lu Z, Tian G, Huang Z, Li Z, Yao J, Luo Q 2017 J. Mater. Chem. C 5 7317 Google Scholar
[12]	Peng Z, Liu Y, Chen K, Yang G, Chen W 2014 Chem. Eng. J. 244 335 Google Scholar
[13]	Zhang M, Jing Y, Zhang J, Sheng Z, Hou Y, Xu J, Chen B, Liu J, Wang M, Hou X 2022 Interdiscip. Mater. 1 157 Google Scholar
[14]	高小钦, 卓宁泽, 王海波, 崔一平, 张家雨 2015 物理学报 64 137801 Google Scholar Gao X Q, Zhuo N Z, Wang H B, Cui Y P, Zhang J Y 2015 Acta Phys. Sin. 64 137801 Google Scholar
[15]	Liu L, Li H, Liu Z, Xie Y H 2018 Mater. Des. 149 145 Google Scholar
[16]	Wang H, Yan X 2019 Phys. Status Solidi-Rapid Res. Lett. 13 1900073 Google Scholar
[17]	Lee Y C, Tsai C C, Liou Y C, Hong C S, Chu S Y 2021 ECS J. Solid State Sci. Technol. 10 063010 Google Scholar
[18]	Onlaor K, Thiwawong T, Tunhoo B 2014 Org. Electron. 15 1254 Google Scholar
[19]	Ma Z, Wu C, Lee D U, Li F, Kim T W 2016 Org. Electron. 28 20 Google Scholar
[20]	Zhang X G, Pantelides S T 2012 Phys. Rev. Lett. 108 266602 Google Scholar
[21]	Feng Y, Lin S, Huang S, Shrestha S, Conibeer G 2015 J. Appl. Phys. 117 125701 Google Scholar
[22]	Durruthy-Rodríguez M, Gervacio-Arciniega J, Hernández-García M, Yáñez-Limón J 2018 J. Adv. Ceram. 7 109 Google Scholar
[23]	邵雅洁, 沈杰, 龚少康, 陈文, 周静 2020 无机化学学报 36 2093 Google Scholar Shao Y J, Shen J, Gong S K, Chen W, Zhou J 2020 Inorg. Chim. Acta. 36 2093 Google Scholar
[24]	Adamu B I, Falak A, Tian Y, Tan X, Meng X, Chen P, Wang H, Chu W 2020 ACS Appl. Mater. Interfaces 12 8411 Google Scholar
[25]	郝国强, 张瑞, 张文静, 陈娜, 叶晓军, 李红波 2022 物理学报 71 017104 Google Scholar Hao G Q, Zhang R, Zhang W J, Chen N, Ye X J, Li H B 2022 Acta Phys. Sin. 71 017104 Google Scholar

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Resistive properties of CuInS₂ quantum dots regulated by niobium-doped lead zirconate titanate ferroelectric films

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

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Resistive properties of CuInS2 quantum dots regulated by niobium-doped lead zirconate titanate ferroelectric films

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

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Resistive properties of CuInS₂ quantum dots regulated by niobium-doped lead zirconate titanate ferroelectric films