Non‐volatile resistive switching (NVRS) is a widely available effect in transitional metal oxides, colloquially known as memristors, and of broad interest for memory technology and neuromorphic computing. Until recently, NVRS was not known in other transitional metal dichalcogenides (TMDs), an important material class owing to their atomic thinness enabling the ultimate dimensional scaling. Here, various monolayer or few‐layer 2D materials are presented in the conventional vertical structure that exhibit NVRS, including TMDs (MX2, M
2D materials have been of considerable interest as new materials for device applications. Non‐volatile resistive switching applications of MoS2and WS2have been previously demonstrated; however, these applications are dramatically limited by high temperatures and extended times needed for the large‐area synthesis of 2D materials on crystalline substrates. The experimental results demonstrate a one‐step sulfurization method to synthesize MoS2and WS2at 550
- Award ID(s):
- 1720595
- NSF-PAR ID:
- 10362511
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Electronic Materials
- Volume:
- 8
- Issue:
- 2
- ISSN:
- 2199-160X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract = transitional metal, e.g., Mo, W, Re, Sn, or Pt; X= chalcogen, e.g., S, Se, or Te), TMD heterostructure (WS2/MoS2), and an atomically thin insulator (h‐BN). These results indicate the universality of the phenomenon in 2D non‐conductive materials, and feature low switching voltage, large ON/OFF ratio, and forming‐free characteristic. A dissociation–diffusion–adsorption model is proposed, attributing the enhanced conductance to metal atoms/ions adsorption into intrinsic vacancies, a conductive‐point mechanism supported by first‐principle calculations and scanning tunneling microscopy characterizations. The results motivate further research in the understanding and applications of defects in 2D materials. -
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Abstract 2D memristors have demonstrated attractive resistive switching characteristics recently but also suffer from the reliability issue, which limits practical applications. Previous efforts on 2D memristors have primarily focused on exploring new material systems, while damage from the metallization step remains a practical concern for the reliability of 2D memristors. Here, the impact of metallization conditions and the thickness of MoS2films on the reliability and other device metrics of MoS2‐based memristors is carefully studied. The statistical electrical measurements show that the reliability can be improved to 92% for yield and improved by ≈16× for average DC cycling endurance in the devices by reducing the top electrode (TE) deposition rate and increasing the thickness of MoS2films. Intriguing convergence of switching voltages and resistance ratio is revealed by the statistical analysis of experimental switching cycles. An “effective switching layer” model compatible with both monolayer and few‐layer MoS2, is proposed to understand the reliability improvement related to the optimization of fabrication configuration and the convergence of switching metrics. The Monte Carlo simulations help illustrate the underlying physics of endurance failure associated with cluster formation and provide additional insight into endurance improvement with device fabrication optimization.
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By mimicking biomimetic synaptic processes, the success of artificial intelligence (AI) has been astounding with various applications such as driving automation, big data analysis, and natural-language processing.[1-4] Due to a large quantity of data transmission between the separated memory unit and the logic unit, the classical computing system with von Neumann architecture consumes excessive energy and has a significant processing delay.[5] Furthermore, the speed difference between the two units also causes extra delay, which is referred to as the memory wall.[6, 7] To keep pace with the rapid growth of AI applications, enhanced hardware systems that particularly feature an energy-efficient and high-speed hardware system need to be secured. The novel neuromorphic computing system, an in-memory architecture with low power consumption, has been suggested as an alternative to the conventional system. Memristors with analog-type resistive switching behavior are a promising candidate for implementing the neuromorphic computing system since the devices can modulate the conductance with cycles that act as synaptic weights to process input signals and store information.[8, 9]
The memristor has sparked tremendous interest due to its simple two-terminal structure, including top electrode (TE), bottom electrode (BE), and an intermediate resistive switching (RS) layer. Many oxide materials, including HfO2, Ta2O5, and IGZO, have extensively been studied as an RS layer of memristors. Silicon dioxide (SiO2) features 3D structural conformity with the conventional CMOS technology and high wafer-scale homogeneity, which has benefited modern microelectronic devices as dielectric and/or passivation layers. Therefore, the use of SiO2as a memristor RS layer for neuromorphic computing is expected to be compatible with current Si technology with minimal processing and material-related complexities.
In this work, we proposed SiO2-based memristor and investigated switching behaviors metallized with different reduction potentials by applying pure Cu and Ag, and their alloys with varied ratios. Heavily doped p-type silicon was chosen as BE in order to exclude any effects of the BE ions on the memristor performance. We previously reported that the selection of TE is crucial for achieving a high memory window and stable switching performance. According to the study which compares the roles of Cu (switching stabilizer) and Ag (large switching window performer) TEs for oxide memristors, we have selected the TE materials and their alloys to engineer the SiO2-based memristor characteristics. The Ag TE leads to a larger memory window of the SiO2memristor, but the device shows relatively large variation and less reliability. On the other hand, the Cu TE device presents uniform gradual switching behavior which is in line with our previous report that Cu can be served as a stabilizer, but with small on/off ratio.[9] These distinct performances with Cu and Ag metallization leads us to utilize a Cu/Ag alloy as the TE. Various compositions of Cu/Ag were examined for the optimization of the memristor TEs. With a Cu/Ag alloying TE with optimized ratio, our SiO2based memristor demonstrates uniform switching behavior and memory window for analog switching applications. Also, it shows ideal potentiation and depression synaptic behavior under the positive/negative spikes (pulse train).
In conclusion, the SiO2memristors with different metallization were established. To tune the property of RS layer, the sputtering conditions of RS were varied. To investigate the influence of TE selections on switching performance of memristor, we integrated Cu, Ag and Cu/Ag alloy as TEs and compared the switch characteristics. Our encouraging results clearly demonstrate that SiO2with Cu/Ag is a promising memristor device with synaptic switching behavior in neuromorphic computing applications.
Acknowledgement This work was supported by the U.S. National Science Foundation (NSF) Award No. ECCS-1931088. S.L. and H.W.S. acknowledge the support from the Improvement of Measurement Standards and Technology for Mechanical Metrology (Grant No. 22011044) by KRISS.
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et al. , Physica Status Solidi (RRL) - Rapid Research Letters, pssr.202200075R1, In press, 2022. -
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Abstract Ferroelectric (FE) devices are conventionally switched by an application of an electric field. However, the recent discoveries of light–matter interactions in heterostructures based on 2D semiconductors and FE materials open new opportunities for using light as an additional tool for device programming. Recently, a purely optical switching of FE polarization in heterostructures comprising 2D MoS2and FE oxide perovskites, such as BaTiO3and Pb(Zr,Ti)O3(PZT), was demonstrated. In this work, it is investigated whether this optical switching has a practical value and can be used to improve functional characteristics of MoS2‐PZT FE field‐effect transistors for nonvolatile memory applications. It is demonstrated that the combined use of an electrical field and visible light improves the nonvolatile ON/OFF ratios in MoS2‐PZT memories by several orders of magnitude compared to their purely electrical operation. The memories are read at zero gate voltage (
V G) in darkness, but their ON and OFF currents, which routinely varied for different devices by over 105, are achieved by programming at the sameV G = −6 V with (ON state) and without (OFF state) light illumination, demonstrating its crucial importance. The light can likely serve as an important tool for better programming of a large variety of other semiconductor‐FE devices. -
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Abstract Au‐mediated exfoliation of 2D transition‐metal dichalcogenides (TMDs) has received significant attention due to its ability to produce large‐area monolayer (ML) flakes. This process has been attributed to strong TMD/Au binding energy (BE) as well as the uniform strain between the TMDs and Au. However, large‐area exfoliation of TMDs with other metals that have even stronger theoretical BE than Au/TMD is not successful, leading to question whether the BE plays any role in the exfoliation process. Here, successful demonstration of large‐area ML MoS2using Cu, Ni, and Ag with various predicted strain, including Pd with almost no strain, but stronger BE than Au/MoS2is demonstrated. Optical micrographs show MoS2flakes with 100s of µm in size with a yield of several tens to hundreds of ML flakes per exfoliation. Photoluminescence and Raman spectroscopy confirm the ML nature of the flakes, while electrical transport measurements show mobilities of
≈ 6 cm2 V−1 s−1with a current on‐off ratio≈ 108consistent with high‐quality ML MoS2. Given that MoS2can be exfoliated with metals that have strong BE irrespective of their strain values suggests that BE is the primary mechanism in successful exfoliation of large‐area ML MoS2.
