Resistive switching behavior of solution-processed AlOx and GO based RRAM at low temperature

https://doi.org/10.1016/j.sse.2019.107735Get rights and content

Abstract

This paper reports on resistive switching behavior observed in resistive random access memory (RRAM) devices fabricated with aluminum oxide (AlOx) and graphene oxide (GO) dielectric films, which were solution-processed under low annealing temperatures of 250 °C and 50 °C for AlOx and GO dielectric films, respectively. As representative of metal oxide and two-dimensional material, a detailed study and comprehensive comparison in view of resistive switching performance has been conducted for AlOx and GO based RRAM, including operation voltage, resistance distribution, resistance ratio, conduction mechanism and retention/endurance property. A smaller operation voltage and better stability were demonstrated in AlOx based RRAM devices while higher resistance magnitude of high resistance state (HRS) and resistance ratio were observed in GO based RRAM devices. The current study opens up promising applications of environmental-friendly solution-processed AlOx and GO films with lower energy consumption for non-volatile memory (NVM).

Introduction

There are theoretical limitations observed in conventional memories like relatively slow operation speed [1], lack of flexibility [2] and low scalability [3]. As a potential replacement for next-generation non-volatile memories (NVM), resistive random access memory (RRAM) devices based on resistive switching (RS) behavior have received considerable attention in recent years. In order to reduce power consumption, accelerate data processing and increase storage density, a large variety of solid-state materials have been investigated as storage medium for RRAM device applications, including metal oxides such as NiOx, TiOx and AlOx [4], [5], [6], [7], [8], [9], organics [10], [11], [12], complex perovskite oxides [13], [14], [15], [16] and carbon-based materials [17], [18], [19]. In particular, metal oxides and carbon-based materials are currently extensively discussed due to the material simplicity [20], [21], [22].

Among various metal oxide based materials, AlOx has attracted considerable attention as dielectric layer with advantages of high dielectric constant (~8), superior elasticity, high toughness and high thermal stability with Si and Pt [23], [24], [25], [26], [27], [28], which shows a great potential as RS layer. Apart from the research on metal oxides, carbon-based materials, as an important class of materials anticipated to overcome the technological barriers of conventional semiconductor electronics, have also been explored extensively in recent years [29], [30], [31]. Related research on carbon-based materials applied in the field effect transistor (FET) devices [32], [33] indicate that it is highly important to investigate their memory behavior as well. Among carbon-based materials, graphene oxide (GO) has been actively investigated having advantages such as, easy synthesis process, nanometer-level scaling down and compatibility for flexible device applications [34], [35], [36]. He et al. has been the first to report reliable and reproducible RS performance of GO thin films deposited by vacuum filtration method [37]. Following on from this study, a large amount of publications have reported on high ON/OFF ratio in the GO based RRAM devices [38], [39], revealing the potential of using GO in RRAM devices. Several fabrication methods such as, atomic-layer-deposition (ALD) [22], [40], [41], [42], magnetron sputtering [43], [44], vacuum filtration [45], [46] and solution-processed (SP) methods [47], [48] have been reported to achieve good performance of RRAM devices. Compared to traditional methods, the solution-processing such as drop casting [49], dip coating [50] and spin coating [47] have considerable appeal due to advantages of low fabrication cost, easy operation and high fabrication efficiency [47], [48], [49], [50].

In this work, the solution-processed dielectrics were fabricated at low annealing temperatures of 250 °C for AlOx film and 50 °C for GO film, and formed the Al/TiN/AlOx/Pt and Al/GO/Si/Al RRAM devices, respectively. A detailed study of RS performance for Al/TiN/AlOx/Pt and Al/GO/Si/Al RRAM devices have been conducted, including operation voltage/resistance distribution, retention and endurance properties. A smaller operation voltage and better stability were demonstrated in AlOx-based RRAM devices while higher resistance of high resistance state (HRS) and higher resistance ratio were observed in GO-based RRAM devices. In addition, the conduction mechanisms of RRAM devices were studied and found to be trap-assisted space-charge-limited conduction (SCLC) in Al/TiN/AlOx/Pt devices and Frenkel-Poole emission in Al/GO/Si/Al devices.

Section snippets

Al/TiN/AlOx/Pt device

The Pt (200 nm)/Ti/SiO2/Si substrates as the bottom electrode (BE) were cleaned with an air plasma system (PDC-002 HARRICK PLASMA expanded plasma cleaner). ~18.76 g of aluminum nitrate nonahydrate (Al (NO3)3·9H2O) was dissolved in 20 mL of deionized water to produce an AlOx precursor solution. Before spin-coating, the mixture was stirred vigorously for 30 min under air ambient conditions and filtered by 0.45 μm polyethersulfone (PES) syringe filters. Then the prepared solution was spin-coated

Results and discussion

The typical DC sweep response of the Al/TiN/AlOx/Pt and Al/GO/Si/Al RRAM devices with 1 mA and 5 mA compliance currents (CC) are plotted in Fig. 2. Both AlOx and GO samples exhibit a reproducible and reversible resistive switching behavior after a electroforming operation with higher voltage. Bistable switching operation between high resistance state (HRS) and low resistance state (LRS) can be observed from the I-V DC sweep characteristics. The arrows in Fig. 2 indicate the directions of

Conclusion

In conclusion, an analysis in light of the switching behavior has been conducted on the solution-processed AlOx and GO dielectrics in RRAM devices prepared under low temperatures. The Al/TiN/AlOx/Pt samples exhibited smaller SET/RESET voltages, HRS resistance and resistance ratio in comparison to Al/GO/Si/Al samples. The conduction mechanisms in the ON and OFF states of the Al/TiN/AlOx/Pt and Al/GO/Si/Al RRAM devices are found to be the SCLC mechanism and Frenkel-Poole emission, respectively.

Acknowledgment

This research was funded in part by the National Natural Science Foundation of China (21503169, 2175011441, and 61704111), Key Program Special Fund in XJTLU (KSF-P-02, KSF-A-04, KSF-A-05, KSF-A-07 and KSF-T-03). The author IZM acknowledges UKRI GIAA award as well as British Council UKIERI project no. IND/CONT/G/17-18/18.

References (58)

  • M. Neumann et al.

    Stable crack propagation in free standing thermal sprayed Al2O3 and Al2O3/ZrO2/TiO2 coatings

    Ceram Int

    (2019)
  • M.-Q. Sun et al.

    Microstructures and mechanical characterizations of high-performance nacre-inspired Al/Al2O3 composites

    Compos A Appl Sci Manuf

    (2019)
  • M.J. Garnier et al.

    Ni-Al2O3 nacre-like composites through hot-pressing of freeze-cast foams

    Mater Sci Eng A

    (2019)
  • T. Nomura et al.

    Al/Al2O3 core/shell microencapsulated phase change material for high-temperature applications

    Sol Energy Mater Sol Cells

    (2019)
  • D. Suh

    Thermal stability of Al2O3/TiO2 stacks for boron emitter passivation on n-type silicon solar cells

    Thin Solid Films

    (2019)
  • S.-Y. Son et al.

    Field effect in amorphous carbon nanomesh directly synthesized from phase-separated polymer blends

    Carbon

    (2019)
  • T. Liu et al.

    Fabrication of carboxymethyl cellulose and graphene oxide bio-nanocomposites for flexible nonvolatile resistive switching memory devices

    Carbohydr Polym

    (2019)
  • B. Ku et al.

    Interface engineering of ALD HfO2-based RRAM with Ar plasma treatment for reliable and uniform switching behaviors

    J Alloy Compd

    (2018)
  • W.Y. Park et al.

    Improvement of sensing margin and reset switching fail of RRAM

    Solid State Electron

    (2019)
  • B. Qi et al.

    57Fe Mössbauer study of epitaxial TiN thin film grown on MgO (100) by magnetron sputtering

    Appl Surf Sci

    (2019)
  • S.M. Islam et al.

    Graphene based material as a base catalyst for solvent free Aldol condensation and Knoevenagel reaction at room temperature

    J Mol Catal A: Chem

    (2014)
  • C.-W. Zhong et al.

    Effect of ITO electrode with different oxygen contents on the electrical characteristics of HfOx RRAM devices

    Surf Coat Technol

    (2013)
  • T.-W. Kim et al.

    Resistive switching characteristics of solution-processed Al–Zn–Sn–O films annealed by microwave irradiation

    Solid State Electron

    (2018)
  • D.B. Strukov et al.

    The missing memristor found

    Nature

    (2008)
  • P. Kumar et al.

    Cross-point resistive switching memory and urea sensing by using annealed GdOxFilm in IrOx/GdOx/W structure for biomedical applications

    J Electrochem Soc

    (2017)
  • S.J. Pearton et al.

    “A review of Ga2O3 materials, processing, and devices,” Applied

    Physics Reviews

    (2018)
  • S.K. Hee-Dong Kim et al.

    Self-rectifying resistive switching behavior observed Al2O3-based resistive switching memory devices with p-AlGaN semiconductor bottom electrode

    J Alloy Compd

    (2018)
  • Z. Sun et al.

    Built-in-homojunction-dominated intrinsically rectifying-resistive switching in NiO nanodots for selection-device-free memory application

    Adv Electron Mater

    (2017)
  • Z. Sun et al.

    Deterministic role of concentration surplus of cation vacancy over anion vacancy in bipolar memristive NiO

    ACS Appl Mater Interfaces

    (2016)
  • Cited by (18)

    • Artificial synapses enabled neuromorphic computing: From blueprints to reality

      2022, Nano Energy
      Citation Excerpt :

      The typical responses to external stimuli are considered to be STP and LTP. When repeated training and rehearsal methods are used, STP, which is connected to the short-term reaction and perception of external stimuli, can transition to LTP [102,103]. Long-term learning and memorization are connected to LTP and are based on the core STP activities.

    • Performance variation of solution-processed memristor induced by different top electrode

      2021, Solid-State Electronics
      Citation Excerpt :

      The same performance could be also observed during the RESET process. For both Ni/AlOx/Pt and TiN/AlOx/Pt RRAM devices, the bipolar RS performance was associated with the switching mechanism based on the formation and rupture of CF in the solution-processed AlOx layer [5,8,10–13,17–24,26–29]. Compared with active metal materials like Ag and Cu, Ni and TiN have lower metal activity, which indicated that the redox reaction of Ni and TiN is not easy to occur during the SET and RESET process [12,13,22–24].

    • Photo-induced switching operations of DNA biopolymer devices

      2021, Functional Materials Processing for Switchable Device Modulation
    View all citing articles on Scopus
    1

    These authors contributed equally to this work.

    View full text