Attachable and flexible aluminum oxide resistive non-volatile memory arrays fabricated on tape as the substrate.

We fabricated 8 × 8 arrays of non-volatile resistive memory devices on commercially available Scotch® Magic™ tape as a flexible substrate. The memory devices consist of double active layers of Al2O3 with a structure of Au/Al2O3/Au/Al2O3/Al (50 nm/20 nm/20 nm/20 nm/50 nm) on attachable tape substrates. Because the memory devices were fabricated using only dry and low temperature processes, the tape substrate did not suffer from any physical or chemical damage during the fabrication. The fabricated memory devices were turned to the low resistance state at ∼3.5 V and turned to the high resistance state at ∼10 V with a negative differential resistance region after ∼5 V, showing typical unipolar non-volatile resistive memory behavior. The memory devices on the tape substrates exhibited reasonable electrical performances including a high ON/OFF ratio of 104, endurance over 200 cycles of reading/writing processes, and retention times of over 104 s in both the flat and bent configurations.

Gate-dependent asymmetric transport characteristics in pentacene barristors with graphene electrodes.

We investigated the electrical characteristics and the charge transport mechanism of pentacene vertical hetero-structures with graphene electrodes. The devices are composed of vertical stacks of silicon, silicon dioxide, graphene, pentacene, and gold. These vertical heterojunctions exhibited distinct transport characteristics depending on the applied bias direction, which originates from different electrode contacts (graphene and gold contacts) to the pentacene layer. These asymmetric contacts cause a current rectification and current modulation induced by the gate field-dependent bias direction. We observed a change in the charge injection barrier during variable-temperature current-voltage characterization, and we also observed that two distinct charge transport channels (thermionic emission and Poole-Frenkel effect) worked in the junctions, which was dependent on the bias magnitude.

Gate-bias stress-dependent photoconductive characteristics of multi-layer MoS2 field-effect transistors.

We investigated the photoconductive characteristics of molybdenum disulfide (MoS2) field-effect transistors (FETs) that were fabricated with mechanically exfoliated multi-layer MoS2 flakes. Upon exposure to UV light, we observed an increase in the MoS2 FET current because of electron-hole pair generation. The MoS2 FET current decayed after the UV light was turned off. The current decay processes were fitted using exponential functions with different decay characteristics. Specifically, a fast decay was used at the early stages immediately after turning off the light to account for the exciton relaxation, and a slow decay was used at later stages long after turning off the light due to charge trapping at the oxygen-related defect sites on the MoS2 surface. This photocurrent decay phenomenon of the MoS2 FET was influenced by the measurement environment (i.e., vacuum or oxygen environment) and the electrical gate-bias stress conditions (positive or negative gate biases). The results of this study will enhance the understanding of the influence of environmental and measurement conditions on the optical and electrical properties of MoS2 FETs.

3D-integrated multilayered physical reservoir array for learning and forecasting time-series information.

A wide reservoir computing system is an advanced architecture composed of multiple reservoir layers in parallel, which enables more complex and diverse internal dynamics for multiple time-series information processing. However, its hardware implementation has not yet been realized due to the lack of a high-performance physical reservoir and the complexity of fabricating multiple stacks. Here, we achieve a proof-of-principle demonstration of such hardware made of a multilayered three-dimensional stacked 3 × 10 × 10 tungsten oxide memristive crossbar array, with which we further realize a wide physical reservoir computing for efficient learning and forecasting of multiple time-series data. Because a three-layer structure allows the seamless and effective extraction of intricate three-dimensional local features produced by various temporal inputs, it can readily outperform two-dimensional based approaches extensively studied previously. Our demonstration paves the way for wide physical reservoir computing systems capable of efficiently processing multiple dynamic time-series information.

Oxygen environmental and passivation effects on molybdenum disulfide field effect transistors.

We investigated the effects of passivation on the electrical characteristics of molybdenum disulfide (MoS(2)) field effect transistors (FETs) under nitrogen, vacuum, and oxygen environments. When the MoS(2) FETs were exposed to oxygen, the on-current decreased and the threshold voltage shifted in the positive gate bias direction as a result of electrons being trapped by the adsorbed oxygen at the MoS(2) surface. In contrast, the electrical properties of the MoS(2) FETs changed only slightly in the different environments when a passivation layer was created using polymethyl methacrylate (PMMA). Specifically, the carrier concentration of unpassivated devices was reduced to 6.5 × 10(15) cm(-2) in oxygen from 16.3 × 10(15) cm(-2) in nitrogen environment. However, in PMMA-passivated devices, the carrier concentration remained nearly unchanged in the range of 1-3 × 10(15) cm(-2) regardless of the environment. Our study suggests that surface passivation is important for MoS(2)-based electronic devices.

A Learning-Rate Modulable and Reliable TiOx Memristor Array for Robust, Fast, and Accurate Neuromorphic Computing.

Realization of memristor-based neuromorphic hardware system is important to achieve energy efficient bigdata processing and artificial intelligence in integrated device system-level. In this sense, uniform and reliable titanium oxide (TiOx ) memristor array devices are fabricated to be utilized as constituent device element in hardware neural network, representing passive matrix array structure enabling vector-matrix multiplication process between multisignal and trained synaptic weight. In particular, in situ convolutional neural network hardware system is designed and implemented using a multiple 25 × 25 TiOx memristor arrays and the memristor device parameters are developed to bring global constant voltage programming scheme for entire cells in crossbar array without any voltage tuning peripheral circuit such as transistor. Moreover, the learning rate modulation during in situ hardware training process is successfully achieved due to superior TiOx memristor performance such as threshold uniformity (≈2.7%), device yield (> 99%), repetitive stability (≈3000 spikes), low asymmetry value of ≈1.43, ambient stability (6 months), and nonlinear pulse response. The learning rate modulable fast-converging in situ training based on direct memristor operation shows five times less training iterations and reduces training energy compared to the conventional hardware in situ training at ≈95.2% of classification accuracy.

Flexible Neural Network Realized by the Probabilistic SiOx Memristive Synaptic Array for Energy-Efficient Image Learning.

The human brain's neural networks are sparsely connected via tunable and probabilistic synapses, which may be essential for performing energy-efficient cognitive and intellectual functions. In this sense, the implementation of a flexible neural network with probabilistic synapses is a first step toward realizing the ultimate energy-efficient computing framework. Here, inspired by the efficient threshold-tunable and probabilistic rod-to-rod bipolar synapses in the human visual system, a 16 × 16 crossbar array comprising the vertical form of gate-tunable probabilistic SiOx memristive synaptic barristor utilizing the Si/graphene heterojunction is designed and fabricated. Controllable stochastic switching dynamics in this array are achieved via various input voltage pulse schemes. In particular, the threshold tunability via electrostatic gating enables the efficient in situ alteration of the probabilistic switching activation (PAct ) from 0 to 1.0, and can even modulate the degree of the PAct change. A drop-connected algorithm based on the PAct is constructed and used to successfully classify the shapes of several fashion items. The suggested approach can decrease the learning energy by up to ≈2,116 times relative to that of the conventional all-to-all connected network while exhibiting a high recognition accuracy of ≈93 %.

Run-off election-based decision method for the training and inference process in an artificial neural network.

Generally, the decision rule for classifying unstructured data in an artificial neural network system depends on the sequence results of an activation function determined by vector-matrix multiplication between the input bias signal and the analog synaptic weight quantity of each node in a matrix array. Although a sequence-based decision rule can efficiently extract a common feature in a large data set in a short time, it can occasionally fail to classify similar species because it does not intrinsically consider other quantitative configurations of the activation function that affect the synaptic weight update. In this work, we implemented a simple run-off election-based decision rule via an additional filter evaluation to mitigate the confusion from proximity of output activation functions, enabling the improved training and inference performance of artificial neural network system. Using the filter evaluation selected via the difference among common features of classified images, the recognition accuracy achieved for three types of shoe image data sets reached ~ 82.03%, outperforming the maximum accuracy of ~ 79.23% obtained via the sequence-based decision rule in a fully connected single layer network. This training algorithm with an independent filter can precisely supply the output class in the decision step of the fully connected network.

One-dimensional organic artificial multi-synapses enabling electronic textile neural network for wearable neuromorphic applications.

One-dimensional (1D) devices are becoming the most desirable format for wearable electronic technology because they can be easily woven into electronic (e-) textile(s) with versatile functional units while maintaining their inherent features under mechanical stress. In this study, we designed 1D fiber-shaped multi-synapses comprising ferroelectric organic transistors fabricated on a 100-µm Ag wire and used them as multisynaptic channels in an e-textile neural network for wearable neuromorphic applications. The device mimics diverse synaptic functions with excellent reliability even under 6000 repeated input stimuli and mechanical bending stress. Various NOR-type textile arrays are formed simply by cross-pointing 1D synapses with Ag wires, where each output from individual synapse can be integrated and propagated without undesired leakage. Notably, the 1D multi-synapses achieved up to ~90 and ~70% recognition accuracy for MNIST and electrocardiogram patterns, respectively, even in a single-layer neural network, and almost maintained regardless of the bending conditions.

Highly Reliable Superhydrophobic Protection for Organic Field-Effect Transistors by Fluoroalkylsilane-Coated TiO2 Nanoparticles.

One of the long-standing problems in the field of organic electronics is their instability in an open environment, especially their poor water resistance. For the reliable operation of organic devices, introducing an effective protection layer using organo-compatible materials and processes is highly desirable. Here, we report a facile method for the depositing of an organo-compatible superhydrophobic protection layer on organic semiconductors under ambient conditions. The protection layer exhibiting excellent water-repellent and self-cleaning properties was deposited onto organic semiconductors directly using a dip-coating process in a highly fluorinated solution with fluoroalkylsilane-coated titanium dioxide (TiO2) nanoparticles. The proposed protection layer did not damage the underlying organic semiconductors and had good resistance against mechanical-, thermal-, light-stress-, and water-based threats. The protected organic field-effect transistors exhibited more-reliable electrical properties, even when exposed to strong solvents, due to its superhydrophobicity. This study provides a practical solution with which to enhance the reliability of environmentally sensitive organic semiconductor devices in the natural environment.

Fabrication of Millimeter-Long Carbon Tubular Nanostructures Using the Self-Rolling Process Inherent in Elastic Protein Layers.

Millimeter-long conducting fibers can be fabricated from carbon nanomaterials via a simple method involving the release of a prestrained protein layer. This study shows how a self-rolling process initiated by polymerization of a micropatterned layer of fibronectin (FN) results in the production of carbon nanomaterial-based microtubular fibers. The process begins with deposition of carbon nanotube (CNT) or graphene oxide (GO) particles on the FN layer. Before polymerization, particles are discrete and nonconducting, but after polymerization the carbon materials become entangled to form an interconnected conducting network clad by FN. Selective removal of FN using high-temperature combustion yields freestanding CNT or reduced GO microtubular fibers. The properties of these fibers are characterized using atomic force microscopy and Raman spectroscopy. The data suggest that this method may provide a ready route to rapid design and fabrication of aligned biohybrid nanomaterials potentially useful for future electronic applications.

Trap-mediated electronic transport properties of gate-tunable pentacene/MoS2 p-n heterojunction diodes.

We investigated the trap-mediated electronic transport properties of pentacene/molybdenum disulphide (MoS2) p-n heterojunction devices. We observed that the hybrid p-n heterojunctions were gate-tunable and were strongly affected by trap-assisted tunnelling through the van der Waals gap at the heterojunction interfaces between MoS2 and pentacene. The pentacene/MoS2 p-n heterojunction diodes had gate-tunable high ideality factor, which resulted from trap-mediated conduction nature of devices. From the temperature-variable current-voltage measurement, a space-charge-limited conduction and a variable range hopping conduction at a low temperature were suggested as the gate-tunable charge transport characteristics of these hybrid p-n heterojunctions. Our study provides a better understanding of the trap-mediated electronic transport properties in organic/2-dimensional material hybrid heterojunction devices.

Integration of Flexible and Microscale Organic Nonvolatile Resistive Memory Devices Using Orthogonal Photolithography.

We present the integration of flexible and microscale organic nonvolatile resistive memory devices fabricated in a cross-bar array structure on plastic substrates. This microscale integration was made via orthogonal photolithography method using fluorinated photoresist and solvents and was achieved without causing damage to the underlying organic memory materials. Our flexible microscale organic devices exhibited high ON/OFF ratio (I(ON/I(OFF) > 10(4)) under bending conditions. In addition, the ON and OFF states of our flexible and microscale memory devices were maintained for 10,000 seconds without any serious degradation.

Origin of multi-level switching and telegraphic noise in organic nanocomposite memory devices.

The origin of negative differential resistance (NDR) and its derivative intermediate resistive states (IRSs) of nanocomposite memory systems have not been clearly analyzed for the past decade. To address this issue, we investigate the current fluctuations of organic nanocomposite memory devices with NDR and the IRSs under various temperature conditions. The 1/f noise scaling behaviors at various temperature conditions in the IRSs and telegraphic noise in NDR indicate the localized current pathways in the organic nanocomposite layers for each IRS. The clearly observed telegraphic noise with a long characteristic time in NDR at low temperature indicates that the localized current pathways for the IRSs are attributed to trapping/de-trapping at the deep trap levels in NDR. This study will be useful for the development and tuning of multi-bit storable organic nanocomposite memory device systems.

Enhancement of photodetection characteristics of MoS2 field effect transistors using surface treatment with copper phthalocyanine.

Recently, two-dimensional materials such as molybdenum disulfide (MoS2) have been extensively studied as channel materials for field effect transistors (FETs) because MoS2 has outstanding electrical properties such as a low subthreshold swing value, a high on/off ratio, and good carrier mobility. In this study, we characterized the electrical and photo-responsive properties of MoS2 FET when stacking a p-type organic copper phthalocyanine (CuPc) layer on the MoS2 surface. We observed that the threshold voltage of MoS2 FET could be controlled by stacking the CuPc layers due to a charge transfer phenomenon at the interface. Particularly, we demonstrated that CuPc/MoS2 hybrid devices exhibited high performance as a photodetector compared with the pristine MoS2 FETs, caused by more electron-hole pairs separation at the p-n interface. Furthermore, we found the optimized CuPc thickness (∼2 nm) on the MoS2 surface for the best performance as a photodetector with a photoresponsivity of ∼1.98 A W(-1), a detectivity of ∼6.11 × 10(10) Jones, and an external quantum efficiency of ∼12.57%. Our study suggests that the MoS2 vertical hybrid structure with organic material can be promising as efficient photodetecting devices and optoelectronic circuits.

1/f Noise Scaling Analysis in Unipolar-Type Organic Nanocomposite Resistive Memory.

We studied noise characteristics of a nanocomposite of polyimide (PI) and phenyl-C61-butyric acid methyl ester (PCBM) (denoted as PI:PCBM), a composite for the organic nonvolatile resistive memory material. The current fluctuations were investigated over a bias range that covers various intermediate resistive states and negative differential resistance (NDR) in organic nanocomposite unipolar resistive memory devices. From the analysis of the 1/f(γ) type noises, scaling behavior between the relative noise power spectral density S̃ and resistance R was observed, indicating a percolating behavior. Considering a linear rate equation of the charge trapping-detrapping at traps, the percolation behavior and NDR could be understood by the modulation of the conductive phase fraction φ with an external bias. This study can enhance the understanding of the NDR phenomena in organic nanocomposite unipolar resistive memory devices in terms of the current path formation and the memory switching.

Graphene/Pentacene Barristor with Ion-Gel Gate Dielectric: Flexible Ambipolar Transistor with High Mobility and On/Off Ratio.

High-quality channel layer is required for next-generation flexible electronic devices. Graphene is a good candidate due to its high carrier mobility and unique ambipolar transport characteristics but typically shows a low on/off ratio caused by gapless band structure. Popularly investigated organic semiconductors, such as pentacene, suffer from poor carrier mobility. Here, we propose a graphene/pentacene channel layer with high-k ion-gel gate dielectric. The graphene/pentacene device shows both high on/off ratio and carrier mobility as well as excellent mechanical flexibility. Most importantly, it reveals ambipolar behaviors and related negative differential resistance, which are controlled by external bias. Therefore, our graphene/pentacene barristor with ion-gel gate dielectric can offer various flexible device applications with high performances.

Electrical and Optical Characterization of MoS2 with Sulfur Vacancy Passivation by Treatment with Alkanethiol Molecules.

We investigated the physical properties of molybdenum disulfide (MoS2) atomic crystals with a sulfur vacancy passivation after treatment with alkanethiol molecules including their electrical, Raman, and photoluminescence (PL) characteristics. MoS2, one of the transition metal dichalcogenide materials, is a promising two-dimensional semiconductor material with good physical properties. It is known that sulfur vacancies exist in MoS2, resulting in the n-type behavior of MoS2. The sulfur vacancies on the MoS2 surface tend to form covalent bonds with sulfur-containing groups. In this study, we deposited alkanethiol molecules on MoS2 field effect transistors (FETs) and then characterized the electrical properties of the devices before and after the alkanethiol treatment. We observed that the electrical characteristics of MoS2 FETs dramatically changed after the alkanethiol treatment. We also observed that the Raman and PL spectra of MoS2 films changed after the alkanethiol treatment. These effects are attributed to the thiol (-SH) end groups in alkanethiols bonding at sulfur vacancy sites, thus altering the physical properties of the MoS2. This study will help us better understand the electrical and optical properties of MoS2 and suggest a way of tailoring the properties of MoS2 by passivating a sulfur vacancy with thiol molecules.

Electric stress-induced threshold voltage instability of multilayer MoS2 field effect transistors.

We investigated the gate bias stress effects of multilayered MoS2 field effect transistors (FETs) with a back-gated configuration. The electrical stability of the MoS2 FETs can be significantly influenced by the electrical stress type, relative sweep rate, and stress time in an ambient environment. Specifically, when a positive gate bias stress was applied to the MoS2 FET, the current of the device decreased and its threshold shifted in the positive gate bias direction. In contrast, with a negative gate bias stress, the current of the device increased and the threshold shifted in the negative gate bias direction. The gate bias stress effects were enhanced when a gate bias was applied for a longer time or when a slower sweep rate was used. These phenomena can be explained by the charge trapping due to the adsorption or desorption of oxygen and/or water on the MoS2 surface with a positive or negative gate bias, respectively, under an ambient environment. This study will be helpful in understanding the electrical-stress-induced instability of the MoS2-based electronic devices and will also give insight into the design of desirable devices for electronics applications.