Tri-level resistive switching characteristics and conductive mechanism of HfO2/NiOx/HfO2 stacks

Chen Tao; Zhang Tao; Yin Yuan-Xiang; Xie Yu-Sha; Qiu Xiao-Yan

doi:10.7498/aps.72.20230331

Abstract

With the extensive integration of portable computers and smartphones with “Internet of Things” technology, further miniaturization, high reading/writing speed and big storage capacity are required for the new-generation non-volatile memory devices. Compared with traditional charge memory and magnetoresistive memory, resistive random access memory (RRAM) based on transition metal oxides is one of the promising candidates due to its low power consumption, small footprint, high stack ability, fast switching speed and multi-level storage capacity.Inspired by the excellent resistive switching characteristics of NiO and HfO₂, NiO_x films are deposited by magnetron sputtering on the Pt$\langle111\rangle $ layer and the polycrystalline HfO₂ film, respectively. Their microstructures, resistive switching characteristics and conductive mechanisms are studied. X-ray diffractometer data show the $\langle111\rangle $ preferred orientation for the NiO_x film deposited on the Pt$\langle111\rangle $ layer but the $\langle100\rangle $ preferred one for the film deposited on the polycrystalline HfO₂ layer. X-ray photoelectron depth profile of Ni 2p core level reveals that the NiO_x film is the mixture of oxygen-deficient NiO and Ni₂O₃. NiO_x(111) films show bipolar resistive switching (RS) characteristics with a clockwise current-voltage (I-V) loop, but its ratio of the high resistance to the low resistance (R_H/R_L) is only ~10, and its endurance is also poor. The NiO_x(200)/HfO₂ stack exhibits bipolar RS characteristics with a counterclockwise I-V loop. The R_H/R_L is greater than 10⁴, the endurance is about 10⁴ cycles, and the retention time exceeds 10⁴ s. In the initial stage, the HfO₂/NiO_x(200)/HfO₂ stack shows similar bi-level RS characteristics to the NiO_x(200)/HfO₂ stack. However, in the middle and the last stages, its I-V curves gradually evolve into tri-level RS characteristics with a “two-step Setting process” in the positive voltage region, showing potential applications in multilevel nonvolatile memory devices and brain-like neural synapses. Its I-V curves in the high and the low resistance state follow the relationship of ohmic conduction ($ I \propto V $), while the I-V curves in the intermediate resistance state are dominated by the space-charge-limited-current mechanism ($ I \propto V^2 $). The tri-level RS phenomena are attributed to the coexistence of the oxygen-vacancy conductive filaments in the NiO_x(200) film and the space charge limited current in the upper HfO₂ film.

Keywords:

Authors and contacts

1.
School of Physical Science and Technology, Southwest University, Chongqing 400715, China
2.
Chongqing Key Laboratory of Micro & Nano Structure Optoelectronics, Southwest University, Chongqing 400715, China

Corresponding author: Qiu Xiao-Yan, qxy2001@swu.edu.cn

Funds: Project supported by the Natural Science Foundation of Chongqing, China (Grant No. cstc2019jcyj-msxm X0451).

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References

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[4]	朱玮, 郭恬恬, 刘兰, 周荣荣 2021 70 068502 Google Scholar Zhu W, Guo T T, Liu L, Zhou R R 2021 Acta Phys. Sin. 70 068502 Google Scholar
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[6]	Wang G Y, Hu L, Xia Y D, Li Q, Xu Q Y 2020 J. Magn. Magn. Mater. 493 165728 Google Scholar
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图 1 (a) Ag/HfO₂/NiO_x/HfO₂/Pt-Si堆栈器件结构示意图; (b) 沉积在Pt-Si衬底上的NiO_x薄膜, NiO_x/HfO₂和HfO₂/NiO_x/HfO₂堆栈样品的XRD谱

Figure 1. (a) Schematic diagram of the Ag/HfO₂/NiO_x/HfO₂/Pt-Si stack; (b) XRD spectra of the NiO_x film, NiO_x/HfO₂ and HfO₂/NiO_x/HfO₂ stacks on Pt coated Si (Pt-Si) substrates.

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图 2 择优取向的(a) NiO_x$\langle111\rangle $和(b) NiO_x$\langle100\rangle $薄膜SEM照片和粒径分布统计图(右上插图)

Figure 2. Top-view SEM images and particle size distributions (upper-right insets) of NiO_x films with the preferred (a) $\langle111\rangle $ and (b) $\langle100\rangle $ orientations, respectively.

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图 3 HfO₂/NiO_x/HfO₂堆栈样品横截面的(a) SEM照片, (b) EDS面扫描总谱以及(c) Ni, (d) O, (e) Pt和(f) Si元素的面分布图. 图(b)中插图为Ni, O, Pt和Hf元素的原子百分含量柱状图

Figure 3. (a) Cross-sectional SEM image, (b) EDS spectrum, and EDS maps of (c) Ni, (d) O, (e) Pt and (f) Si elements for the HfO₂/NiO_x/HfO₂ stack on the Pt-Si substrate. Inset in Fig.(b) shows the atomic percent of Ni, O, Pt, and Hf elements in the sample.

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图 4 (a) 沉积在Pt-Si衬底上的HfO₂/NiO_x/HfO₂堆栈横截面的HRTEM照片; 图(a)中的(b) HfO₂/NiO_x界面局部区域(红色方框标注)和(c) NiO_x/HfO₂/Pt局部区域(白色方框标注)的高倍数HRTEM照片

Figure 4. (a) HRTEM images for the cross sectional HfO₂/NiO_x/HfO₂ stack on Pt-Si substrate. Magnified HRTEM images for (b) the HfO₂/NiO_x and (c) the NiO_x/HfO₂/Pt interfaces marked with the red and the white boxes in Fig.(a), respectively.

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图 5 HfO₂/NiO_x/HfO₂堆栈中Hf, Ni, Pt和O的原子百分含量随刻蚀次数的变化

Figure 5. Variations of the atomic percent for Hf, Ni, Pt, and O in the HfO₂/NiO_x/HfO₂ stack with etching times.

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图 6 HfO₂/NiO_x/HfO₂堆栈样品的(a) Pt 4f, (b) Hf 4f和(c) Ni 2p核心能级的XPS深度剖析谱

Figure 6. XPS depth profiles of (a) Pt 4f, (b) Hf 4f and (c) Ni 2p core levels for the HfO₂/NiO_x/HfO₂ stack.

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图 7 P1, P2和P3峰面积百分比随刻蚀次数的变化

Figure 7. Variations of the peak area percentage for P1, P2, and P3 sub-peaks with etching times.

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图 8 HfO₂/NiO_x/HfO₂堆栈器件的电阻开关特性　(a) I-V回线; (b) 0.1 V电压读取的高电阻态, 中间电阻态和低电阻态阻值随循环周期数的变化; (c) V_Set1, V_Set2和V_Reset的累积概率分布以及(d) 器件在高(低)电阻态的持续时间

Figure 8. Resistive switching properties of the HfO₂/NiO_x/HfO₂ stack: (a) I-V loops; (b) variations of resistance for the HRS, IRS and LRS with the cycle number at the reading voltage of 0.1 V; (c) cumulative probability distributions of V_Set1, V_Set2 and V_Reset; (d) retention time of the HRS and the LRS.

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图 9 (a), (b) NiO_x薄膜, (c), (d) NiO_x/HfO₂和(e)—(h) HfO₂/NiO_x/HfO₂堆栈在对数-线性坐标中的I-V回线及其在双对数坐标中绘制的Set过程附近的I-V曲线

Figure 9. I-V loops in logarithmic-linear scale and replotted I-V curves in double-logarithmic scale near the Set process of RRAM cells based on (a), (b) NiO_x films, (c), (d) NiO_x/HfO₂ and (e)–(h) HfO₂/NiO_x/HfO₂ stacks, respectively.

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图 10 HfO₂/NiO_x/HfO₂堆栈器件电阻开关微观机制示意图　(a) 扩散过程; (b) Set1过程; (c) Set2过程; (d) Reset过程

Figure 10. Schematic illustrations of the resistive switching mechanism for the HfO₂/NiO_x/HfO₂ stack in the (a) diffusion; (b) Set1; (c) Set2 and (d) Reset processes

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表 1 Ag/HfO₂/NiO_x/HfO₂/Pt堆栈器件的制备工艺参数

Table 1. Preparation parameters of the Ag/HfO₂/NiO_x/HfO₂/Pt stack.

成分	溅射源 (99.99％纯度)	生长气氛流量(比)	衬底温度/℃	溅射方式功率/W, 偏压/V	生长时间/min	退火气氛流量(比)	退火温度/℃	退火时间/min
Pt金属层	Pt金属靶	2.7 Pa Ar+O₂ Ar∶O₂ = 17∶3	700	直流 25, 0	5	—	—	—
HfO₂薄膜	HfO₂陶瓷靶	3 Pa Ar 30 sccm	350	射频 70, 0	20	3 Pa O₂ 30 sccm	350	30
NiO_x薄膜	Ni金属靶	0.5 Pa Ar+O₂ Ar∶O₂ = 4∶1	700	射频 60, 0	90	0.5 Pa Ar+O₂ Ar∶O₂ = 4∶1	700	30
Ag电极	Ag金属靶	0.5 Pa Ar 30 sccm	250	直流 25, –100	10	—	—	—
注: sccm为cm³/min.

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表 2 各种氧化物/NiO_x堆栈RRAM器件的电阻开关性能参数

Table 2. Resistive switching parameters of RRAM cells based on various oxide/NiO_x stacks.

Cell structure	Switching type	V_Set/V	V_Reset/V	R_H/R_L	Endurance	Retention/s	Ref.
NiFe/Al₂O₃/NiO/Pt	Unipolar	2.30—4.20	0.55—1.50	～1×10³	>1×10²	1×10⁴	[6]
Pt/IrO₂/NiO/IrO₂/Pt	Unipolar	1.43	0.41	> 1×10²	2×10²	—	[19]
Ag/HfO₂/NiO/Pt	Bipolar	0.20	–0.20	> 1×10³	> 5×10³	> 1×10³	[20]
Pt/NiO/Mg_0.6Zn_0.4O/Pt	Rectifying	—	0.54—0.62	～1×10⁶	1×10²	6×10⁴	[21]
Au/BaTiO₃/NiO/Pt	Unipolar	2.00	1.00	—	—	—	[22]
Ag/HfO₂/nb-NiO/Pt	Bipolar	0.16—0.38	–0.19— –0.38	～1×10⁴	1.2×10³	>1×10⁴	[28]
Pt/BiFeO₃/NiO/Pt	Bipolar	1.00—1.50	–0.20— –0.60	> 10	30	—	[33]
Ag/NiO_x/HfO₂/Pt	Bipolar	0.12—0.18	–0.02— –0.17	> 1×10⁴	～1×10⁴	> 1×10⁴	Reference cell
Ag/HfO₂/NiO_x/HfO₂/Pt	Bipolar	Set1: 0.13—0.17	–0.03— –0.17	～1×10⁵	> 3×10³	～1×10⁴	This work
Ag/HfO₂/NiO_x/HfO₂/Pt	Bipolar	Set2: 0.21—0.40	–0.03— –0.17	～1×10²	> 3×10³	～1×10⁴	This work

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map

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[2]	Zhou G D, Ji X Y, Li J, Zhou F C, Dong Z K, Yan B T, Sun B, Wang W H, Hu X F, Song Q L, Wang L D, Duan S K 2022 iScience 25 105240 Google Scholar
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[4]	朱玮, 郭恬恬, 刘兰, 周荣荣 2021 70 068502 Google Scholar Zhu W, Guo T T, Liu L, Zhou R R 2021 Acta Phys. Sin. 70 068502 Google Scholar
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[6]	Wang G Y, Hu L, Xia Y D, Li Q, Xu Q Y 2020 J. Magn. Magn. Mater. 493 165728 Google Scholar
[7]	Xia W Y, Sun X W, Yin Y F, Jia C H, Li G Q, Zhang W F 2020 AIP Adv. 10 105319 Google Scholar
[8]	Chu J X, Li Y, Fan X H, Shao H H, Duan W J, Pei Y L 2018 Semicond. Sci. Technol. 33 115007 Google Scholar
[9]	Jung K, Choi J, Kim Y, Im H, Seo S, Jung R, Kim D, Kim J S, Park B H, Hong J P 2008 J. Appl. Phys. 103 034504 Google Scholar
[10]	Yuan X C, Wei X H, Dai B, Zeng H Z 2016 Appl. Surf. Sci. 362 506 Google Scholar
[11]	D'Aquila K, Liu Y Z, Iddir H, Petford-Long A K 2015 Phys. Status Solidi RRL 9 301 Google Scholar
[12]	Lee S, Kim D, Eom H, Kim W B, Yoo B 2014 Jpn. J. Appl. Phys. 53 024202 Google Scholar
[13]	Ge N N, Gong C H, Yuan X C, Zeng H Z, Wei X H 2018 RSC Adv. 8 29499 Google Scholar
[14]	Li J C, Hou X Y, Cao Q 2014 J. Appl. Phys. 115 164507 Google Scholar
[15]	Kim J, Na H, Lee S, Sung Y H, Yoo J H, Lee D S, Ko D H, Sohn H 2011 Curr. Appl. Phys. 11 e70 Google Scholar
[16]	Kim J, Lee K, Sohn H 2009 J. Electrochem. Soc. 156 H881 Google Scholar
[17]	Ma G K, Tang X L, Zhang H W, Zhong Z Y, Li X, Li J, Su H 2017 J. Mater. Sci. 52 238 Google Scholar
[18]	Huang Y C, Chen P Y, Chin T S, Liu R S, Huang C Y, Lai C H 2012 Appl. Phys. Lett. 101 153106 Google Scholar
[19]	Kim D C, Lee M J, Ahn S E, Seo S, Park J C, Yoo I K, Beak I G, Kim H J, Yim E K, Lee J E, Park S O, Kim H S, Chung U I, Moon J T, Ryu B I 2006 Appl. Phys. Lett. 88 232106 Google Scholar
[20]	Qiu X Y, Wang R X, Zhang Z, Wei M L, Ji H, Chai Y, Zhou F C, Dai J Y, Zhang T, Li L T, Meng X S 2017 Appl. Phys. Lett. 111 142103 Google Scholar
[21]	Chen X M, Zhou H, Wu G H, Bao D H 2011 Appl. Phys. A-Mater. Sci. Process. 104 477 Google Scholar
[22]	Li S, Wei X H, Lei Y, Yuan X C, Zeng H Z 2016 Appl. Surf. Sci. 389 977 Google Scholar
[23]	Zhang T, Zhang Z, Chan C H, Li L T, Wei M L, Meng X S, Dai J Y, Qiu X Y 2018 J. Phys. D: Appl. Phys. 51 305105 Google Scholar
[24]	Banerjee W, Kashir A, Kamba S 2022 Small 18 2107575 Google Scholar
[25]	Park M, Jeon B, Park J, Kim S 2022 Nanomaterials 12 4206 Google Scholar
[26]	Chen Y J, Chang K C, Chang T C, Chen H L, Young T F, Tsai T M, Zhang R, Chu T J, Ciou J F, Lou J C, Chen K H, Chen J H, Zheng J C, Sze S M 2014 IEEE Electron Device Lett. 35 1016 Google Scholar
[27]	Yan X Y, Wang X T, Wang D, et al. 2020 Nanotechnology 31 115209 Google Scholar
[28]	Yin Y X, Xie Y S, Chen T, Xiang Y J, Zhou K, Qiu X Y 2023 Appl. Surf. Sci. 613 155994 Google Scholar
[29]	Qiu X Y, Wang R X, Li G Q, et al. 2017 Appl. Surf. Sci. 406 212 Google Scholar
[30]	Kim K S, Winograd N 1974 Surf. Sci. 43 625 Google Scholar
[31]	Khan M Q, Ahmad K, Alsalme A, Kim H 2022 Mater. Chem. Phys. 289 126463 Google Scholar
[32]	Smolarek M, Kierzkowska-Pawlak H, Kapica R, Fronczak M, Sitarz M, Lesniak M, Tyczkowski J 2021 Catalysts 11 905 Google Scholar
[33]	Luo J M, Zhang H N, Chen S H, Yang X D, Bu S L, Wen J P 2016 Chem. Phys. Lett. 652 98 Google Scholar
[34]	潘峰, 陈超 2014 阻变存储器材料与器件 (北京: 科学出版社) 第43页 Pan F, Chen C 2014 Resistive Random Access Memory Materials and Devices (Beijing: Science Press) p43 (in Chinese)
[35]	Sze S M, Ng K K 2007 Physics of Semiconductor Devices (3rd Ed.) (America: John Wiley & Sons, Inc.) p227
[36]	Siddik A, Halder P K, Garu P, et al. 2020 J. Phys. D: Appl. Phys. 53 295103 Google Scholar
[37]	Li Y, Fang P W, Fan X H, Pei Y L 2020 Semicond. Sci. Technol. 35 055004 Google Scholar
[38]	Zhang W, Lei J Z, Dai Y X, Zhang X H, Kang L M, Peng B W, Hu F R 2022 Nanotechnology 33 255703 Google Scholar
[39]	Li Z H, Li J C, Cui H P 2021 J. Alloys Compd. 858 158091 Google Scholar
[40]	Ismail M, Chand U, Mahata C, Nebhen J, Kim S 2022 J. Mater. Sci. Technol. 96 94 Google Scholar
[41]	Wang W, Covi E, Lin Y H, et al. 2021 IEEE Trans. Electron Devices 68 4342 Google Scholar
[42]	Hong D S, Wang W X, Chen Y S, Sun J R, Shen B G 2014 Appl. Phys. Lett. 105 113504 Google Scholar
[43]	Yuan F, Shen S S, Zhang Z G, Pan L Y, Xu J 2016 Superlattices Microstruct. 91 90 Google Scholar
[44]	Razi P M, Angappane S, Gangineni R B 2021 Mater. Sci. Eng. B-Adv. 263 114852 Google Scholar
[45]	Sun B, Zhang X J, Zhou G D, Yu T, Mao S S, Zhu S H, Zhao Y, Xia Y D 2018 J. Colloid Interface Sci. 520 19 Google Scholar

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Vol. 72, Issue 14 - 2023-07-20

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Tri-level resistive switching characteristics and conductive mechanism of HfO₂/NiO_x/HfO₂ stacks

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Corresponding author: Qiu Xiao-Yan, qxy2001@swu.edu.cn

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