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

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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 HfO ₂, NiO _xfilms are deposited by magnetron sputtering on the Pt $\langle111\rangle $ layer and the polycrystalline HfO ₂film, respectively. Their microstructures, resistive switching characteristics and conductive mechanisms are studied. X-ray diffractometer data show the $\langle111\rangle $ preferred orientation for the NiO _xfilm deposited on the Pt $\langle111\rangle $ layer but the $\langle100\rangle $ preferred one for the film deposited on the polycrystalline HfO ₂layer. X-ray photoelectron depth profile of Ni 2p core level reveals that the NiO _xfilm is the mixture of oxygen-deficient NiO and Ni ₂O ₃. 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)/HfO ₂stack exhibits bipolar RS characteristics with a counterclockwise I-Vloop. The R _H/ R _Lis greater than 10 ⁴, the endurance is about 10 ⁴cycles, and the retention time exceeds 10 ⁴s. In the initial stage, the HfO ₂/NiO _x(200)/HfO ₂stack shows similar bi-level RS characteristics to the NiO _x(200)/HfO ₂stack. However, in the middle and the last stages, its I-Vcurves 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-Vcurves in the high and the low resistance state follow the relationship of ohmic conduction ( $ I \propto V $ ), while the I-Vcurves 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 HfO ₂film.

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

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