Rational Design on Controllable Cation Injection with Improved Conductive-Bridge Random Access Memory by Glancing Angle Deposition Technology toward Neuromorphic Application

A conductive-bridge random access memory (CBRAM) has been considered a promising candidate for the next-generation nonvolatile memory technology because of its excellent performance, for which the resistive switching behavior depends on the formation/dissolution of conducting filaments in an electrolyte layer originated by the cation injection from the active electrode with electrochemical reactions. Typically, the controllability of cations into the electrolyte layer is a main issue, leading to stable switching reliability. In this work, an architecture combining spike-shaped Ag electrodes created by Al2O3 nanopillar arrays as a physical diffusion barrier by glancing angle deposition technology was proposed to localize Ag cation injection for the formation of controllable filaments inside TiOx as the switching layer. Interestingly, the dimension of the Ag plugs defined by the topography of Al2O3 nanopillar arrays can control Ag cation injection to influence the dimensionality of conductive filaments. Compared to the typical planar-Ag/TiOx/Pt device, the spiked-Ag/Al2O3 nanopillar arrays/TiOx/Pt device shows improvement of endurance and voltage disturbance. With enhanced multilevel characteristics, the spiked active-metal-based CBRAM device can be expected to serve as an analogue synapse for neuromorphic applications

Tunable Multilevel Storage of Complementary Resistive Switching on Single-Step Formation of ZnO/ZnWO_<i>x</i> Bilayer Structure via Interfacial Engineering

Tunable multilevel storage of complementary resistive switching (CRS) on single-step formation of ZnO/ZnWO_<i>x</i> bilayer structure via interfacial engineering was demonstrated for the first time. In addition, the performance of the ZnO/ZnWO_<i>x</i>-based CRS device with the voltage- and current-sweep modes was demonstrated and investigated in detail. The resistance switching behaviors of the ZnO/ZnWO_<i>x</i> bilayer ReRAM with adjustable RESET-stop voltages was explained using an electrochemical redox reaction model whose electron-hopping activation energies of 28, 40, and 133 meV can be obtained from Arrhenius equation at RESET-stop voltages of 1.0, 1.3, and 1.5 V, respectively. In the case of the voltage-sweep operation on the ZnO-based CRS device, the maximum array numbers (<i>N</i>) of 9, 15, and 31 at RESET-stop voltages of 1.4, 1.5, and 1.6 V were estimated, while the maximum array numbers increase into 47, 63, and 105 at RESET-stop voltages of 2.0, 2.2, and 2.4 V, operated by the current-sweep mode, respectively. In addition, the endurance tests show a very stable multilevel operation at each RESET-stop voltage under the current-sweep mode

Geometric Design of Confined Conducting Filaments in Resistive Random Access Memory by Al₂O₃ Nanodome-Shaped Arrays (NDSAs) via Glancing-Angle Deposition Technology Toward Neuromorphic Computing

Resistive random access memory (RRAM) is vital to neuromorphic computing applications. However, filamentary RRAM cells are affected by transitions from abrupt switching to analog switching. In this study, we develop Al2O3 nanodome-shaped arrays (NDSAs) by glancing-angle deposition technology (GLAD) to geometrically confine the conducting filaments (CFs), for which conducting atomic force microscopy (C-AFM) was performed to analyze positions and dimensions of filaments. For the Pt/HfO2/75% Al2O3 NDSAs/TiN device, the dimension of the CFs can be restricted to 10–12 nm, whereas for the Pt/HfO2/TiN device, the CFs were formed with a dimension of ∼50 nm. The device first yielded multiple weak CFs that subsequently transformed to stronger and larger CFs when the coverage of Al2O3 NDSAs was reduced to 55% while Pt/HfO2/75% Al2O3 NDSAs/TiN device exhibited synaptic features with more linear potentiation and depression, demonstrating the analog switching. The controllable coverages of Al2O3 NDSAs render the geometric design more promising as a memristor for future applications in neuromorphic computing

Direct Synthesis of Graphene with Tunable Work Function on Insulators via In Situ Boron Doping by Nickel-Assisted Growth

Work function engineering, a precise tuning of the work function, is essential to achieve devices with the best performance. In this study, we demonstrate a simple technique to deposit graphene on insulators with in situ controlled boron doping to tune the work function. At a temperature higher than 1000 °C, the boron atoms substitute carbon sites in the graphene lattice with neighboring carbon atoms, leading to the graphene with a p-type doping behavior. Interestingly, the involvement of boron vapor into the system can effectively accelerate the reaction between nickel vapor and methane, achieving a fast graphene deposition. The changes in surface potential and work function at different doping levels were verified by Kelvin probe force microscopy, for which the work function at different doping levels was shifted between 20 and 180 meV. Finally, the transport mechanism followed by the Mott variable-range hopping model was found due to the strong disorder nature of the system with localized charge-carrier states

Single CuO_<i>x</i> Nanowire Memristor: Forming-Free Resistive Switching Behavior

CuO_<i>x</i> nanowires were synthesized by a low-cost and large-scale electrochemical process with AAO membranes at room temperature and its resistive switching has been demonstrated. The switching characteristic exhibits forming-free and low electric-field switching operation due to coexistence of significant amount of defects and Cu nanocrystals in the partially oxidized nanowires. The detailed resistive switching characteristics of CuO_<i>x</i> nanowire systems have been investigated and possible switching mechanisms are systematically proposed based on the microstructural and chemical analysis via transmission electron microscopy

Selection Role of Metal Oxides into Transition Metal Dichalcogenide Monolayers by a Direct Selenization Process

Direct reduction of metal oxides into a few transition metal dichalcogenide (TMDCs) monolayers has been recently explored as an alternative method for large area and uniform deposition. However, not many studies have addressed the characteristics and requirement of the metal oxides into TMDCs by the selenization/sulfurization processes, yielding a wide range of outstanding properties to poor electrical characteristics with nonuniform films. The large difference implies that the process is yet not fully understood. In particular, the selenization/sulfurization at low temperature leads to poor crystallinity films with poor electrical performance, hindering its practical development. A common approach to improve the quality of the selenized/sulfurized films is by further increasing the process temperature, thus requiring additional transfer in order to explore the electrical properties. Here, we show that by finely tuning the quality of the predeposited oxide the selenization/sulfurization temperature can be largely decreased, avoiding major substrate damage and allowing direct device fabrication. The direct relationship between the role of selecting different metal oxides prepared by e-beam evaporation and reactive sputtering and their oxygen deficiency/vacancy leading to quality influence of TMDCs was investigated in detail. Because of its outstanding physical properties, the formation of tungsten diselenide (WSe2) from the reduction of tungsten oxide (WOx) was chosen as a model for proof of concept. By optimizing the process parameters and the selection of metal oxides, layered WSe2 films with controlled atomic thickness can be demonstrated. Interestingly, the domain size and electrical properties of the layered WSe2 films are highly affected by the quality of the metal oxides, for which the layered WSe2 film with small domains exhibits a metallic behavior and the layered WSe2 films with larger domains provides clear semiconducting behavior. Finally, an 8′′ wafer scale-layered WSe2 film was demonstrated, giving a step forward in the development of 2D TMDC electronics in the industry

Rational Design on Polymorphous Phase Switching in Molybdenum Diselenide-Based Memristor Assisted by All-Solid-State Reversible Intercalation toward Neuromorphic Application

In this work, a low-power memristor based on vertically stacked two-dimensional (2D) layered materials, achieved by plasma-assisted vapor reaction, as the switching material, with which the copper and gold metals as electrodes featured by reversible polymorphous phase changes from a conducting 1T-phase to a semiconducting 2H-one once copper cations interacted between vertical lamellar layers and vice versa, was demonstrated. Here, molybdenum diselenide was chosen as the switching material, and the reversible polymorphous phase changes activated by the intercalation of Cu cations were confirmed by pseudo-operando Raman scattering, transmission electron microscopy, and scanning photoelectron microscopy under high and low resistance states, respectively. The switching can be activated at about ±1 V with critical currents less than 10 μA with an on/off ratio approaching 100 after 100 cycles and low power consumption of ∼0.1 microwatt as well as linear weight updates controlled by the amount of intercalation. The work provides alternative feasibility of reversible and all-solid-state metal interactions, which benefits monolithic integrations of 2D materials into operative electronic circuits

Design of Mixed-Dimensional QDs/MoS₂/TiO₂ Heterostructured Resistive Random-Access Memory with Interfacial Analog Switching Characteristics for Potential Neuromorphic Computing

Resistive random-access memory (RRAM) is one of the most promising candidates for next-generation nanoscale nonvolatile memory devices and neuromorphic computing applications. In this study, we developed a novel mixed-dimensional design for RRAM devices, incorporating zero-dimensional quantum dots (QDs), two-dimensional MoS2, and a TiO2 switching layer to achieve prominent interfacial switching behaviors. Compared with typical filamentary RRAM devices, the proposed heterostructure featured a light-sensitive QDs/MoS2 layer that allowed for bias-controllable resistive changes during the set and reset processes without abrupt switching. This was endowed by effective electron–hole pair separations upon excitation and the generation of a thin molybdenum oxide (MoOx) layer due to the accumulation of oxygen ions at the interface between MoS2 and TiO2. The ITO/QDs/MoS2/TiO2/Pt RRAM device exhibited an on/off ratio of 10 with improved endurance under 515 nm laser illumination and wavelength-dependent resistive switching behavior, making it useful for multilevel storage. Furthermore, the heterostructured device demonstrated synaptic characteristics with enhanced potentiation and depression nonlinearities and asymmetry factors, revealing its potential for future neuromorphic applications

Environmentally and Mechanically Stable Selenium 1D/2D Hybrid Structures for Broad-Range Photoresponse from Ultraviolet to Infrared Wavelengths

Selenium (Se) is one of the potential candidates as photodetector because of its outstanding properties such as high photoconductivity (∼8 × 104 S cm–1), piezoelectricity, thermoelectricity, and nonlinear optical responses. Solution phase synthesis becomes an efficient way to produce Se, but a contamination issue that could deteriorate the electric characteristic of Se should be taken into account. In this work, a facile, controllable approach of synthesizing Se nanowires (NWs)/films via a plasma-assisted growth process was demonstrated at the low substrate temperature of 100 °C. The detailed formation mechanisms of nanowires arrays to thin films at different plasma powers were investigated. Moreover, indium (In) layer was used to enhance the adhesive strength with 50% improvement on a SiO2/Si substrate by mechanical interlocking and surface alloying between Se and In layers, indicating great tolerance for mechanical stress for future wearable devices applications. Furthermore, the direct growth of Se NWs/films on a poly­(ethylene terephthalate) substrate was demonstrated, exhibiting a visible to broad infrared detection ranges from 405 to 1555 nm with a high on/off ratio of ∼700 as well as the fast response time less than 25 ms. In addition, the devices exhibited fascinating stability in the atmosphere over one month

Environmentally and Mechanically Stable Selenium 1D/2D Hybrid Structures for Broad-Range Photoresponse from Ultraviolet to Infrared Wavelengths

Selenium (Se) is one of the potential candidates as photodetector because of its outstanding properties such as high photoconductivity (∼8 × 104 S cm–1), piezoelectricity, thermoelectricity, and nonlinear optical responses. Solution phase synthesis becomes an efficient way to produce Se, but a contamination issue that could deteriorate the electric characteristic of Se should be taken into account. In this work, a facile, controllable approach of synthesizing Se nanowires (NWs)/films via a plasma-assisted growth process was demonstrated at the low substrate temperature of 100 °C. The detailed formation mechanisms of nanowires arrays to thin films at different plasma powers were investigated. Moreover, indium (In) layer was used to enhance the adhesive strength with 50% improvement on a SiO2/Si substrate by mechanical interlocking and surface alloying between Se and In layers, indicating great tolerance for mechanical stress for future wearable devices applications. Furthermore, the direct growth of Se NWs/films on a poly­(ethylene terephthalate) substrate was demonstrated, exhibiting a visible to broad infrared detection ranges from 405 to 1555 nm with a high on/off ratio of ∼700 as well as the fast response time less than 25 ms. In addition, the devices exhibited fascinating stability in the atmosphere over one month