Photo-Assisted Ferroelectric Domain Control for α-In2Se3 Artificial Synapses Inspired by Spontaneous Internal Electric Fields.

α-In2Se3 semiconductor crystals realize artificial synapses by tuning in-plane and out-of-plane ferroelectricity with diverse avenues of electrical and optical pulses. While the electrically induced ferroelectricity of α-In2Se3 shows synaptic memory operation, the optically assisted synaptic plasticity in α-In2Se3 has also been preferred for polarization flipping enhancement. Here, the synaptic memory behavior of α-In2Se3 is demonstrated by applying electrical gate voltages under white light. As a result, the induced internal electric field is identified at a polarization flipped conductance channel in α-In2Se3/hexagonal boron nitride (hBN) heterostructure ferroelectric field effect transistors (FeFETs) under white light and discuss the contribution of this built-in electric field on synapse characterization. The biased dipoles in α-In2Se3 toward potentiation polarization direction by an enhanced internal built-in electric field under illumination of white light lead to improvement of linearity for long-term depression curves with proper electric spikes. Consequently, upon applying appropriate electric spikes to α-In2Se3/hBN FeFETs with illuminating white light, the recognition accuracy values significantly through the artificial learning simulation is elevated for discriminating hand-written digit number images.

Increased Mobility and Reduced Hysteresis of MoS2 Field-Effect Transistors via Direct Surface Precipitation of CsPbBr3-Nanoclusters for Charge Transfer Doping.

Transition-metal dichalcogenides (TMDs) and metal halide perovskites (MHPs) have been investigated for various applications, owing to their unique physical properties and excellent optoelectronic functionalities. TMD monolayers synthesized via chemical vapor deposition (CVD), which are advantageous for large-area synthesis, exhibit low mobility and prominent hysteresis in the electrical signals of field-effect transistors (FETs) because of their native defects. In this study, we demonstrate an increase in electrical mobility by ∼170 times and reduced hysteresis in the current-bias curves of MoS2 FETs hybridized with CsPbBr3 for charge transfer doping, which is implemented via solution-based CsPbBr3-nanocluster precipitation on CVD-grown MoS2 monolayer FETs. Electrons injected from CsPbBr3 into MoS2 induce heavy n-doping and heal point defects in the MoS2 channel layer, thus significantly increasing mobility and reducing hysteresis in the hybrid FETs. Our results provide a foundation for improving the reliability and performance of TMD-based FETs by hybridizing them with solution-based perovskites.

Reliable synaptic plasticity of InGaZnO transistor with TiO2interlayer.

We demonstrate an InGaZnO (IGZO)-based synaptic transistor with a TiO2buffer layer. The structure of the synaptic transistor with TiO2inserted between the Ti metal electrode and an IGZO semiconductor channel O2trapping layer produces a large hysteresis window, which is crucial for achieving synaptic functionality. The Ti/TiO2/IGZO synaptic transistor exhibits reliable synaptic plasticity features such as excitatory post-synaptic current, paired-pulse facilitation, and potentiation and depression, originating from the reversible charge trapping and detrapping in the TiO2layer. Finally, the pattern recognition accuracy of Modified National Institute of Standards and Technology handwritten digit images was modeled using CrossSim simulation software. The simulation results present a high image recognition accuracy of ∼89%. Therefore, this simple approach using an oxide buffer layer can aid the implementation of high-performance synaptic devices for neuromorphic computing systems.

In-depth analysis on electrical parameters of floating gate IGZO synaptic transistor affecting pattern recognition accuracy.

The reliable conductance modulation of synaptic devices is key when implementing high-performance neuromorphic systems. Herein, we propose a floating gate indium gallium zinc oxide (IGZO) synaptic device with an aluminum trapping layer to investigate the correlation between its diverse electrical parameters and pattern recognition accuracy. Basic synaptic properties such as excitatory postsynaptic current, paired pulse facilitation, long/short term memory, and long-term potentiation/depression are demonstrated in the IGZO synaptic transistor. The effects of pulse tuning conditions associated with the pulse voltage magnitude, interval, duration, and cycling number of the applied pulses on the conductance update are systematically investigated. It is discovered that both the nonlinearity of the conductance update and cycle-to-cycle variation should be critically considered using an artificial neural network simulator to ensure the high pattern recognition accuracy of Modified National Institute of Standards and Technology (MNIST) handwritten digit images. The highest recognition rate of the MNIST handwritten dataset is 94.06% for the most optimized pulse condition. Finally, a systematic study regarding the synaptic parameters must be performed to optimize the developed synapse device.

In-depth analysis on electrical parameters of floating gate IGZO synaptic transistor affecting pattern recognition accuracy.

The reliable conductance modulation of synaptic devices is key when implementing high-performance neuromorphic systems. Herein, we propose a floating gate IGZO synaptic device with an aluminum trapping layer to investigate the correlation between its diverse electrical parameters and pattern recognition accuracy. Basic synaptic properties such as excitatory postsynaptic current, paired pulse facilitation, long/short term memory, and long-term potentiation/depression are demonstrated in the IGZO synaptic transistor. The effects of pulse tuning conditions associated with the pulse voltage magnitude, interval, duration, and cycling number of the applied pulses on the conductance update are systematically investigated. It is discovered that both the nonlinearity of the conductance update and cycle-to-cycle variation should be critically considered using an artificial neural network simulator to ensure the high pattern recognition accuracy of Modified National Institute of Standards and Technology (MNIST) handwritten digit images. The highest recognition rate of the MNIST handwritten dataset is 94.06% for the most optimized pulse condition. Finally, a systematic study regarding the synaptic parameters must be performed to optimize the developed synapse device.

Accelerated Learning in Wide-Band-Gap AlN Artificial Photonic Synaptic Devices: Impact on Suppressed Shallow Trap Level.

Artificial synaptic platforms are promising for next-generation semiconductor computing devices; however, state-of-the-art optoelectronic approaches remain challenging, owing to their unstable charge trap states and limited integration. We demonstrate wide-band-gap (WBG) III-V materials for photoelectronic neural networks. Our experimental analysis shows that the enhanced crystallinity of WBG synapses promotes better synaptic characteristics, such as effective multilevel states, a wider dynamic range, and linearity, allowing the better power consumption, training, and recognition accuracy of artificial neural networks. Furthermore, light-frequency-dependent memory characteristics suggest that artificial optoelectronic synapses with improved crystallinity support the transition from short-term potentiation to long-term potentiation, implying a clear emulation of the psychological multistorage model. This is attributed to the charge trapping in deep-level states and suppresses fast decay and nonradiative recombination in shallow traps. We believe that the fingerprints of these WBG synaptic characteristics provide an effective strategy for establishing an artificial optoelectronic synaptic architecture for innovative neuromorphic computing.

One-step H2S reactive sputtering for 2D MoS2/Si heterojunction photodetector.

A technique for directly growing two-dimensional (2D) materials onto conventional semiconductor substrates, enabling high-throughput and large-area capability, is required to realise competitive 2D transition metal dichalcogenide devices. A reactive sputtering method based on H2S gas molecules and sequential in situ post-annealing treatment in the same chamber was proposed to compensate for the relatively deficient sulfur atoms in the sputtering of MoS2 and then applied to a 2D MoS2/p-Si heterojunction photodevice. X-ray photoelectron, Raman, and UV-visible spectroscopy analysis of the as-deposited Ar/H2S MoS2 film were performed, indicating that the stoichiometry and quality of the as-deposited MoS2 can be further improved compared with the Ar-only MoS2 sputtering method. For example, Ar/H2S MoS2 photodiode has lower defect densities than that of Ar MoS2. We also determined that the factors affecting photodetector performance can be optimised in the 8-12 nm deposited thickness range.

Facile fabrication of ZnO nanowire memory device based on chemically-treated surface defects.

In this study, we demonstrate a transistor-type ZnO nanowire (NW) memory device based on the surface defect states of a rough ZnO NW, which is obtained by introducing facile H2O2 solution treatment. The surface defect states of the ZnO NW are validated by photoluminescence characterisation. A memory device based on the rough ZnO NW exhibits clearly separated bi-stable states (ON and OFF states). A significant current fluctuation does not exist during repetitive endurance cycling test. Stable memory retention characteristics are also achieved at a high temperature of 85 °C and at room temperature. The surface-treated ZnO NW device also exhibits dynamically well-responsive pulse switching under a sequential pulse test configuration, thereby indicating its potential practical memory applications. The simple chemical treatment strategy can be widely used for modulating the surface states of diverse low-dimensional materials.

Enhanced Performance of MoS2 Photodetectors by Inserting an ALD-Processed TiO2 Interlayer.

2D molybdenum disulfide (MoS2 ) possesses excellent optoelectronic properties that make it a promising candidate for use in high-performance photodetectors. Yet, to meet the growing demand for practical and reliable MoS2 photodetectors, the critical issue of defect introduction to the interface between the exfoliated MoS2 and the electrode metal during fabrication must be addressed, because defects deteriorate the device performance. To achieve this objective, the use of an atomic layer-deposited TiO2 interlayer (between exfoliated MoS2 and electrode) is reported in this work, for the first time, to enhance the performance of MoS2 photodetectors. The TiO2 interlayer is inserted through 20 atomic layer deposition cycles before depositing the electrode metal on MoS2 /SiO2 substrate, leading to significantly enhanced photoresponsivity and response speed. These results pave the way for practical applications and provide a novel direction for optimizing the interlayer material.

Self-Formed Channel Devices Based on Vertically Grown 2D Materials with Large-Surface-Area and Their Potential for Chemical Sensor Applications.

2D layered materials with sensitive surfaces are promising materials for use in chemical sensing devices, owing to their extremely large surface-to-volume ratios. However, most chemical sensors based on 2D materials are used in the form of laterally defined active channels, in which the active area is limited to the actual device dimensions. Therefore, a novel approach for fabricating self-formed active-channel devices is proposed based on 2D semiconductor materials with very large surface areas, and their potential gas sensing ability is examined. First, the vertical growth phenomenon of SnS2 nanocrystals is investigated with large surface area via metal-assisted growth using prepatterned metal electrodes, and then self-formed active-channel devices are suggested without additional pattering through the selective synthesis of SnS2 nanosheets on prepatterned metal electrodes. The self-formed active-channel device exhibits extremely high response values (>2000% at 10 ppm) for NO2 along with excellent NO2 selectivity. Moreover, the NO2 gas response of the gas sensing device with vertically self-formed SnS2 nanosheets is more than two orders of magnitude higher than that of a similar exfoliated SnS2 -based device. These results indicate that the facile device fabrication method would be applicable to various systems in which surface area plays an important role.

Alloyed 2D Metal-Semiconductor Heterojunctions: Origin of Interface States Reduction and Schottky Barrier Lowering.

The long-term stability and superior device reliability through the use of delicately designed metal contacts with two-dimensional (2D) atomic-scale semiconductors are considered one of the critical issues related to practical 2D-based electronic components. Here, we investigate the origin of the improved contact properties of alloyed 2D metal-semiconductor heterojunctions. 2D WSe2-based transistors with mixed transition layers containing van der Waals (M-vdW, NbSe2/WxNb1-xSe2/WSe2) junctions realize atomically sharp interfaces, exhibiting long hot-carrier lifetimes of approximately 75,296 s (78 times longer than that of metal-semiconductor, Pd/WSe2 junctions). Such dramatic lifetime enhancement in M-vdW-junctioned devices is attributed to the synergistic effects arising from the significant reduction in the number of defects and the Schottky barrier lowering at the interface. Formation of a controllable mixed-composition alloyed layer on the 2D active channel would be a breakthrough approach to maximize the electrical reliability of 2D nanomaterial-based electronic applications.

Alloyed 2D Metal-Semiconductor Atomic Layer Junctions.

Heterostructures of compositionally and electronically variant two-dimensional (2D) atomic layers are viable building blocks for ultrathin optoelectronic devices. We show that the composition of interfacial transition region between semiconducting WSe2 atomic layer channels and metallic NbSe2 contact layers can be engineered through interfacial doping with Nb atoms. WxNb1-xSe2 interfacial regions considerably lower the potential barrier height of the junction, significantly improving the performance of the corresponding WSe2-based field-effect transistor devices. The creation of such alloyed 2D junctions between dissimilar atomic layer domains could be the most important factor in controlling the electronic properties of 2D junctions and the design and fabrication of 2D atomic layer devices.

Electrohydrodynamic printing for scalable MoS2 flake coating: application to gas sensing device.

Scalable sub-micrometer molybdenum disulfide ([Formula: see text]) flake films with highly uniform coverage were created using a systematic approach. An electrohydrodynamic (EHD) printing process realized a remarkably uniform distribution of exfoliated [Formula: see text] flakes on desired substrates. In combination with a fast evaporating dispersion medium and an optimal choice of operating parameters, the EHD printing can produce a film rapidly on a substrate without excessive agglomeration or cluster formation, which can be problems in previously reported liquid-based continuous film methods. The printing of exfoliated [Formula: see text] flakes enabled the fabrication of a gas sensor with high performance and reproducibility for [Formula: see text] and [Formula: see text].

Low interfacial contact resistance of Al-graphene composites via interface engineering.

Al-based composites incorporating multilayered graphene sheets were developed via a facile approach. The multilayered graphene sheets were fabricated from the expanded graphite via a simple mechanical exfoliation process. The facile extrusion molding process with Al powder and graphene sheets exfoliated from expended graphite afforded Al-based graphene composite rods. These composites showed enhanced thermal conductivity compared to the pristine Al rods. Moreover, the Al-based multilayered graphene sheet composites exhibited lower interfacial contact resistance between graphene-based electrodes than the pristine Al. With increasing degrees of dispersion, the number of exposed graphene sheets increases, thereby significantly decreasing the interfacial contact resistance between the composite and external graphite electrode.

Metal Decoration Effects on the Gas-Sensing Properties of 2D Hybrid-Structures on Flexible Substrates.

We have investigated the effects of metal decoration on the gas-sensing properties of a device with two-dimensional (2D) molybdenum disulfide (MoS2) flake channels and graphene electrodes. The 2D hybrid-structure device sensitively detected NO2 gas molecules (>1.2 ppm) as well as NH3 (>10 ppm). Metal nanoparticles (NPs) could tune the electronic properties of the 2D graphene/MoS2 device, increasing sensitivity to a specific gas molecule. For instance, palladium NPs accumulate hole carriers of graphene/MoS2, electronically sensitizing NH3 gas molecules. Contrarily, aluminum NPs deplete hole carriers, enhancing NO2 sensitivity. The synergistic combination of metal NPs and 2D hybrid layers could be also applied to a flexible gas sensor. There was no serious degradation in the sensing performance of metal-decorated MoS2 flexible devices before/after 5000 bending cycles. Thus, highly sensitive and endurable gas sensor could be achieved through the metal-decorated 2D hybrid-structure, offering a useful route to wearable electronic sensing platforms.

Nonvolatile analog memory transistor based on carbon nanotubes and C60 molecules.

A nonvolatile analog memory transistor is demonstrated by integrating C60 molecules as charge storage molecules in the transistor gate, and carbon nanotubes (CNTs) in the transistor channel. The currents through the CNT channel can be tuned quantitatively and reversibly to analog values by controlling the number of electrons trapped in the C60 molecules. After tuning, the electrons trapped in the C60 molecules in the gate, and the current through the CNT channel, can be preserved in a nonvolatile manner, indicating the characteristics of the nonvolatile analog memory.

Conduction Mechanism in Acceptor- or Donor-Doped ZrO2 Bulk and Thin Films.

The leakage current in capacitors in future electronics should be highly suppressed to achieve low power consumption, high reliability, and fast data processing. Although considerable efforts have been directed at reducing the leakage current, fundamental studies on the effects of doping on bulk and thin-film materials have rarely been conducted. Herein, we investigated the effects of doping with acceptor and donor elements on the conduction of bulk and thin-film ZrO2 and elucidated the underlying charge conduction mechanism. In the case of bulk ZrO2, the electrical conductivity was reliably modulated by the type of dopant element, which is highly consistent with defect chemistry theory. However, unlike in the bulk material, in acceptor- and donor-doped thin-film ZrO2, the leakage current was suppressed, indicating that the factors determining the electrical property in thin films are different from those in bulk materials.

Reinforcing Synaptic Plasticity of Defect-Tolerant States in Alloyed 2D Artificial Transistors.

While two-dimensional (2D) materials possess the desirable future of neuromorphic computing platforms, unstable charging and de-trapping processes, which are inherited from uncontrollable states, such as the interface trap between nanocrystals and dielectric layers, can deteriorate the synaptic plasticity in field-effect transistors. Here, we report a facile and effective strategy to promote artificial synaptic devices by providing physical doping in 2D transition-metal dichalcogenide nanomaterials. Our experiments demonstrate that the introduction of niobium (Nb) into 2D WSe2 nanomaterials produces charge trap levels in the band gap and retards the decay of the trapped charges, thereby accelerating the artificial synaptic plasticity by encouraging improved short-/long-term plasticity, increased multilevel states, lower power consumption, and better symmetry and asymmetry ratios. Density functional theory calculations also proved that the addition of Nb to 2D WSe2 generates defect tolerance levels, thereby governing the charging and de-trapping mechanisms of the synaptic devices. Physically doped electronic synapses are expected to be a promising strategy for the development of bioinspired artificial electronic devices.

Organic nonvolatile memory devices with charge trapping multilayer graphene film.

We fabricated an array-type organic nonvolatile memory device with multilayer graphene (MLG) film embedded in polyimide (PI) layers. The memory devices showed a high ON/OFF ratio (over 10(6)) and a long retention time (over 10(4) s). The switching of the Al/PI/MLG/PI/Al memory devices was due to the presence of the MLG film inserted into the PI layers. The double-log current-voltage characteristics could be explained by the space-charge-limited current conduction based on a charge-trap model. A conductive atomic force microscopy found that the conduction paths in the low-resistance ON state were distributed in a highly localized area, which was associated with a carbon-rich filamentary switching mechanism.

Highly Reproducible Heterosynaptic Plasticity Enabled by MoS2/ZrO2-x Heterostructure Memtransistor.

Electrically tunable resistive switching of a polycrystalline MoS2-based memtransistor has attracted a great deal of attention as an essential synaptic component of neuromorphic circuitry because its switching characteristics from the field-induced migration of sulfur defects in the MoS2 grain boundaries can realize multilevel conductance tunability and heterosynaptic functionality. However, reproducible switching properties in the memtransistor are usually disturbed by the considerable difficulty in controlling the concentration and distribution of the intrinsically existing sulfur defects. Herein, we demonstrate reliable heterosynaptic characteristics using a memtransistor device with a MoS2/ZrO2-x heterostructure. Compared to the control device with the MoS2 semiconducting channel, the Schottky barrier height was more effectively modulated by the insertion of the insulating ZrO2-x layer below the MoS2, confirmed by an ultraviolet photoelectron spectroscopy analysis and the corresponding energy-band structures. The MoS2/ZrO2-x memtransistor accomplishes dual-terminal (drain and gate electrode) stimulated multilevel conductance owing to the tunable resistive switching behavior under varying gate voltages. Furthermore, the memtransistor exhibits long-term potentiation/depression endurance cycling over 7000 pulses and stable pulse cycling behavior by the pulse stimulus from different terminal regions. The promising candidate as an essential synaptic component of the MoS2/ZrO2-x memtransistors for neuromorphic systems results from the high recognition accuracy (∼92%) of the deep neural network simulation test, based on the training and inference of handwritten numbers (0-9). The simple memtransistor structure facilitates the implementation of complex neural circuitry.