基于1, 2 - 二氰基苯/聚合物复合材料的高耐久性有机阻变存储器

李伟; 朱慧文; 孙彤; 屈文山; 李建刚; 杨辉; 高志翔; 施薇; 魏斌; 王华

doi:10.7498/aps.72.20221507

摘要

本文报道了一种基于1,2-二氰基苯 (O-DCB) 与聚 (3-己基噻吩) (P3HT) 复合薄膜的高耐久性有机阻变存储器 (ORSM). ORSM表现出非易失型和双极性存储特性, 电流开关比 (I_on/off) 超过10⁴, 耐久性高达400次, 保持时间为10⁵ s, V_set和V_reset分别为–6.9 V和2.6 V. 器件的阻变机理是陷阱电荷的俘获与去俘获, 即负偏压或正偏压诱导电荷陷阱的填充和抽离过程, 导致电荷传输方式的改变, 从而产生高低电阻间的切换. 器件的高耐久性一方面是由于O-DCB较小的分子尺寸和较好的溶解性形成了均匀分布且稳定的电荷陷阱, 另一方面是由于O-DCB较好的分子平面促进了其与P3HT共轭链的相互作用. 该研究为高耐久性ORSM的实现提供了一种有效途径, 加快了ORSM的商业化应用进程.

关键词:

Abstract

As the emerging data storage technology, organic resistive switching memory (ORSM) possesses numerous superiorities as the substitution for or the complementation of the traditional Si-based semiconductor memory. Poly(3-hexylthiophene) (P3HT) has been widely used as a polymer donor component of ORSMs due to its advantages of high mobility and high chemical stability. Up to now, ORSM based on P3HT has achieved high on/off current ratio (I_on/off), but the endurance still needs to be improved. Herein, high endurance ORSMs based on 1,2-dicyanobenzene (O-DCB) and P3HT composite are fabricated by spin coating and thermally evaporating, and exhibit non-volatile and bipolar memory characteristics. The ORSMs based on P3HT:15 wt.% O-DCB and P3HT:30 wt.% O-DCB exhibit the values of I_on/off exceeding 10⁴ and 10³ respectively, and both of them exert excellent endurance of 400 times, retention time of more than 10⁵ s. The mechanism of the switching is explored by linear fitting of I-V curve and electrochemical impedance spectrum . The results indicate that the filling and vacant process of the charge traps induced by O-DCB and the inherent traps in P3HT bulk lead to a resistive switching effect. The negative or positive bias triggers off trapping and detrapping process, which leads the conductive way of charges to change, resulting in the resistive switching effect. The excellent endurance of ORSM is attributed to the uniform distribution of O-DCB in P3HT bulk because of the small molecular size and high solubility of O-DCB, resulting in well-distributed and stable charge traps. On the other hand, the out-bound planarity of O-DCB molecular promotes the close interaction with the conjugated chains of P3HT. This study enlightens an effective strategy to carry out high-endurance ORSM and facilitates their electronic applications in future.

Keywords:

作者及机构信息

1.
山西大同大学固体物理研究所, 微结构电磁功能材料省市共建山西省重点实验室, 大同　037009

2.
山西大同大学化学与化工学院, 大同　037009

3.
上海大学机电工程与自动化学院, 新型显示技术及应用集成教育部重点实验室, 上海　200072

4.
上海大学材料科学与工程学院, 上海　200072

5.
太原理工大学, 新材料界面科学与工程教育部重点实验室, 太原　030024

通信作者: 高志翔, 03100012@sxdtdx.edu.cn ; 施薇, shiwei@shu.edu.cn ;

基金项目: 山西省应用基础研究计划面上自然基金(批准号: 201901D111316)、山西省高等学校科技创新项目(批准号: 2020L0488)、大同市工业攻关项目(批准号: 2019015)、山西省研究生教育创新项目(批准号: 2022Y761)和山西大同大学研究生教育创新项目(批准号: 22CX02, 22CX16)资助的课题.

Authors and contacts

1.
Shanxi Province Key Laboratory of Microstructure Functional Materials Institute of Solid State Physics, Shanxi Datong University, Datong 037009, China

2.
School of Chemistry and Chemical Engineering, Shanxi Datong University, Datong 037009, China

3.
Key Laboratory of Advanced Display and System Applications, Ministry of Education, School of Mechatronic Engineering and Automation, Shanghai University, Shanghai 200072, China

4.
School of Materials Science and Engineering, Shanghai University, Shanghai 200072, China

5.
Key Laboratory of Interface Science and Engineering in Advanced Materials, Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, China

Corresponding author: Gao Zhi-Xiang, 03100012@sxdtdx.edu.cn ; Shi Wei, shiwei@shu.edu.cn ;

Funds: Project supported by the Applied Basic Research Project of Shanxi Province (Grant No. 201901D111316), the Science and technology innovation project of Shanxi Colleges and Universities (Grant No. 2020L0488), the Datong City Key Industry Research Project (Grant No. 2019015), the Graduate Education Innovation Project of Shanxi Province (Grant No.2022Y761), and the Graduate Education Innovation Project of Shanxi Datong University (Grant Nos. 22CX02, 22CX16).

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参考文献

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施引文献

图 1 (a) P3HT和O-DCB的分子结构; (b) ORSM器件结构

Fig. 1. (a) Chemical structures of P3HT and O-DCB; (b) schematic diagram of the ORSM.

下载: 全尺寸图片幻灯片

图 2 (a) O-DCB的吸收光谱、激发光谱和发射光谱; P3HT, P3HT: 15% O-DCB和P3HT: 30% O-DCB的 (b) 吸收光谱和 (c) 荧光光谱; P3HT, P3HT: 15% O-DCB, P3HT: 30% O-DCB和P3HT: 45% O-DCB薄膜的AFM形貌图; P3HT: 15% O-DCB和P3HT: 30% O-DCB薄膜S和N元素的分布图

Fig. 2. (a) Absorption, excitation and emission spectra of O-DCB; (b) normalized UV-vis absorption spectra and (c) PL spectra of P3HT, P3HT: 15% O-DCB and P3HT: 30% O-DCB. AFM images of (d) P3HT, (e) P3HT: 15% O-DCB, (f) P3HT: 30% O-DCB, and (g) P3HT: 45% O-DCB films. Distribution maps of S and N elements of (h)(i) P3HT: 15% O-DCB and (j)(k) P3HT: 30% O-DCB films.

下载: 全尺寸图片幻灯片

图 3 (a) P3HT, (b) P3HT: 15% O-DCB, (c) P3HT: 30% O-DCB, (d) P3HT: 45% O-DCB器件的I-V特性; (e) P3HT: 15% O-DCB和 (f) P3HT: 30% O-DCB器件的I_on/off-V特性; (g) P3HT: 15% O-DCB和 (h) P3HT: 30% O-DCB器件的切换速度测试

Fig. 3. I-V characterizations of devices with (a) P3HT, (b) P3HT:15% O-DCB, (c) P3HT:30% O-DCB, and (d) P3HT:45% O-DCB. I_on/off-V characterizations of devices with (e) P3HT:15% O-DCB and (f) P3HT:30% O-DCB. Switching speed test of devices with (g) P3HT:15% O-DCB and (h) P3HT:30% O-DCB.

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图 4 (a)—(c) D1和 (d)—(f) D2的 (a)(d) 耐久性、(b)(e) 保持性和 (c)(f) 脉冲周期、宽度、电压为4 μs、4 μs和–1 V时的读脉冲稳定性测试

Fig. 4. (a)(d) Endurance cycles test, (b)(e) retention time test, and (c)(f) reading pulse test with the pulse period and width of 4 μs and 4 μs and the voltage of –1 V of (a)–(c) D1 and (d)–(f) D2.

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图 5 (a) D1和 (b) D2的I-V曲线的线性拟合结果; (c) P3HT器件以及 (d)(f) D1和 (e)(g) D2分别在(d)(e) LRS和(f)(g) HRS的Nyquist图; (h) 阻抗的虚部与频率关系图

Fig. 5. Linear fitting of the I-V curves of (a) D1 and (b) D2. Nyquist plots of (c) P3HT based device, (d)(f) D1 and (e)(g) D2 in (d)(e) LRS and (f)(g) HRS; (h) plots of the imaginary part of the impedance vs. frequency of devices in LRS.

下载: 全尺寸图片幻灯片

图 6 (a) ORSM的能级结构图; (b)—(f)器件的阻变机理示意图 (b) 陷阱电荷俘获阶段; (c) 陷阱填满阶段; (d) 陷阱电荷去俘获阶段; (e) 空陷阱阶段; (f) 电流泄露

Fig. 6. (a) Energy diagram of the ORSM; (b)–(f) Schematic illustration of the switching mechanism: Charge transfer processes of (b) trap filling, (c) fully filling trap, (d) trap pumping, (e) vacant trap, and (f) current leakage.

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表 1 D1和D2的器件参数汇总

Table 1. Summary of device parameters for D1 and D2.

器件 V_set/V V_reset/V I_on/off 耐久性保持性/s 存储类型

D1 –6.9 2.6 1.5×10⁴ 400 10⁵ Flash
D2 –6.2 2.8 1.0×10³ 400 10⁵ Flash

下载: 导出CSV

[1]	Zhang Z, Wang Z, Shi T, Bi C, Rao F, Cai Y, Liu Q, Wu H, Zhou P 2020 InfoMat 2 261 Google Scholar
[2]	Service R F 2018 Science 361 321 Google Scholar
[3]	Debenedictis E P 2019 Computer 52 114 Google Scholar
[4]	Zahoor F, Azni Zulkifli T Z, Khanday F A 2020 Nanoscale Res. Lett. 15 90 Google Scholar
[5]	Wong H S P, Lee H Y, Yu S, Chen Y S, Wu Y, Chen P S, Lee B, Chen F T, Tsai M J 2012 Proc. IEEE 100 1951 Google Scholar
[6]	Sangwan V K, Lee H S, Bergeron H, Balla I, Beck M E, Chen K S, Hersam M C 2018 Nature 554 500 Google Scholar
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[10]	古亚娜, 梁燕, 王光义, 夏晨阳 2022 物理学报 71 110501 Google Scholar Gu Y N, Liang Y, Wang G Y, Xia C Y 2022 Acta Phys. Sin. 71 110501 Google Scholar
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[12]	Lee J H, Park S P, Park K, Kim H J 2019 Adv. Funct. Mater. 30 1907437
[13]	Gao S, Yi X, Shang J, Liu G, Li R W 2019 Chem. Soc. Rev. 48 1531 Google Scholar
[14]	卢颖, 陈威林, 高双, 李润伟 2020 材料导报 34 1146 Google Scholar Lu Y, Chen W L, Gao S, Li R W 2020 Mat. Rep. 34 1146 Google Scholar
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[29]	Liang J, Su Y, Lin Q, Zhou H, Zhang S, Pei Y, Hu R 2014 Semicond. Sci. Technol. 29 115029 Google Scholar
[30]	Sherazi S S H, Rehman M M, Ur Rehman H M M, Kim W Y, Siddiqui G U, Karimov K S 2020 Semicond. Sci. Technol. 35 125012 Google Scholar
[31]	Sim R, Ming W, Setiawan Y, Lee P S 2012 J. Phys. Chem. C 117 677
[32]	Wang P, Liu Q, Zhang C Y, Jiang J, Wang L H, Chen D Y, Xu Q F, Lu J M 2015 Nanoscale 7 19579 Google Scholar
[33]	丛麟权, 李文骁, 马瑛, 曲旭坡, 邢颖 2020 染料与染色 57 24 Cong L Q, Li W X, Ma Y, Qu X P, Xing Y 2020 Dyestuffs and Coloration 57 24
[34]	王述 1983 辽宁化工 56 Wang S 1983 Liaoning Chem. Ind. 56 (in Chinses)
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[36]	Yuan J, Wang Y, Li L, Wang S, Tang X, Wang H, Li M, Zheng C, Chen R 2020 J. Phys. Chem. C 124 10129 Google Scholar
[37]	Zhang L, Li Y, Shi J, Shi G, Cao S 2013 Mater. Chem. Phys. 142 626 Google Scholar
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[43]	Pan S, Zhu Z, Yu H, Lan W, Wei B, Guo K 2021 J. Mater. Chem. C 9 5643 Google Scholar
[44]	Yamazaki Y, Yamashita K, Tani Y, Aoyama T, Ogawa T 2020 J. Mater. Chem. C 8 14423 Google Scholar
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基于1, 2 - 二氰基苯/聚合物复合材料的高耐久性有机阻变存储器