Harnessing a WOx-based flexible transparent memristor synapse with a hafnium oxide layer for neuromorphic computing.

Transparent memristor-based neuromorphic synapses are expected to be specialised devices for high-speed information transmission and processing. The synaptic linearity and potentiation/depression cycles are imperative issues for the application of memristors. This work explores a memristor for improving switching uniformity by introducing a thin HfOx interfacial layer as a diffusion-limiting layer sandwiched between WOx and ITO bottom electrodes. An optimized HfOx thickness not only provides the best switching properties but also shows superior synaptic properties. The optimized 15 nm thin WOx layer can retain the memristor's excellence in P/D linearity, a cycling stability of 494 epochs and image recognition up to 3 mm bending, making it suitable for flexible devices. The artificial synapse is capable of reversible short-term and long-term learning behaviors confirmed by spike-timing-dependent-plasticity (STDP) results. X-ray photoelectron spectroscopy confirms the device composition and provides the oxygen vacancy concentration at the WOx/HfOx interface to realize the switching mechanism. The thicknesses of the different layers are estimated from the high-resolution transmission electron microscopy observations. The fabricated device exhibits 92.2% transparency, as confirmed by the UV-Vis spectrum.

All oxide based flexible multi-folded invisible synapse as vision photo-receptor.

All oxide-based transparent flexible memristor is prioritized for the potential application in artificially simulated biological optoelectronic synaptic devices. SnOx memristor with HfOx layer is found to enable a significant effect on synaptic properties. The memristor exhibits good reliability with long retention, 104 s, and high endurance, 104 cycles. The optimized 6 nm thick HfOx layer in SnOx-based memristor possesses the excellent synaptic properties of stable 350 epochs training, multi-level conductance (MLC) behaviour, and the nonlinearity of 1.53 and 1.46 for long-term potentiation and depression, respectively, and faster image recognition accuracy of 100% after 23 iterations. The maximum weight changes of -73.12 and 79.91% for the potentiation and depression of the synaptic device, respectively, are observed from the spike-timing-dependent plasticity (STDP) characteristics making it suitable for biological applications. The flexibility of the device on the PEN substrate is confirmed by the acceptable change of nonlinearities up to 4 mm bending. Such a synaptic device is expected to be used as a vision photo-receptor.

CMOS-Compatible Memristor for Optoelectronic Neuromorphic Computing.

Optoelectronic memristor is a promising candidate for future light-controllable high-density storage and neuromorphic computing. In this work, light-tunable resistive switching (RS) characteristics are demonstrated in the CMOS process-compatible ITO/HfO2/TiO2/ITO optoelectronic memristor. The device shows an average of 79.24% transmittance under visible light. After electroforming, stable bipolar analog switching, data retention beyond 104 s, and endurance of 106 cycles are realized. An obvious current increase is observed under 405 nm wavelength light irradiation both in high and in low resistance states. The long-term potentiation of synaptic property can be achieved by both electrical and optical stimulation. Moreover, based on the optical potentiation and electrical depression of conductances, the simulated Hopfield neural network (HNN) is trained for learning the 10 × 10 pixels size image. The HNN can be successfully trained to recognize the input image with a training accuracy of 100% in 13 iterations. These results suggest that this optoelectronic memristor has a high potential for neuromorphic application.

Ion accumulation-induced capacitance elevation in a microporous graphene-based supercapacitor.

High-performance porous 3D graphene-based supercapacitors are one of the most promising and challenging directions for future energy technologies. Microporous graphene has been synthesized by the pyrolysis method. The fabricated lightweight graphene with a few layers (FLG) has an ultra-high surface area of 2266 m2 g-1 along with various-sized micropores. The defect-induced morphology and pore size distribution of the fabricated graphene are examined, and the results show that the micropores vary from 0.85 to 1.9 nm and the 1.02 nm pores contribute 30% of the total surface area. The electrochemical behaviour of the electrode fabricated using this graphene has been studied with various concentrations of the KOH electrolyte. The highest specific capacitance of the graphene electrode of 540 F g-1 (close to the theoretical value, ∼550 F g-1) can be achieved by using the 1 M KOH electrolyte. This high specific capacitance contribution involves the counter ion adsorption, co-ion desorption, and ion permutation mechanisms. The formation of a Helmholtz layer, as well as the diffusion of the electrolyte ions, confirms this phenomenon. The symmetrical solid-state supercapacitor fabricated with the graphene electrodes and PVA-KOH gel as the electrolyte exhibits excellent energy and power densities of 18 W h kg-1 and 10.2 kW kg-1, respectively. This supercapacitor also shows a superior 100% coulombic efficiency after 6000 cycles.

Negative Effects of Annealed Seed Layer on the Performance of ZnO-Nanorods Based Nitric Oxide Gas Sensor.

Nitric oxide (NO) is a toxic gas, which is dangerous for human health and causes many respiratory infections, poisoning, and lung damage. In this work, we have successfully grown ZnO nanorod film on annealed ZnO seed layer in different ambient temperatures, and the morphology of the nanorods sensing layer that affects the gas sensing response to nitric oxide (NO) gas were investigated. To acknowledge the effect of annealing treatment, the devices were fabricated with annealed seed layers in air and argon ambient at 300 °C and 500 °C for 1 h. To simulate a vertical device structure, a silver nanowire electrode covered in ZnO nanorod film was placed onto the hydrothermal grown ZnO nanorod film. We found that annealing treatment changes the seed layer's grain size and defect concentration and is responsible for this phenomenon. The I-V and gas sensing characteristics were dependent on the oxygen defects concentration and porosity of nanorods to react with the target gas. The resulting as-deposited ZnO seed layer shows better sensing response than that annealed in an air and argon environment due to the nanorod morphology and variation in oxygen defect concentration. At room temperature, the devices show good sensing response to NO concentration of 10 ppb and up to 100 ppb. Shortly, these results can be beneficial in the NO breath detection for patients with chronic inflammatory airway disease, such as asthma.

Pentafluoropyridine functionalized novel heteroatom-doped with hierarchical porous 3D cross-linked graphene for supercapacitor applications.

The fabrication with high energy density and superior electrical/electrochemical properties of hierarchical porous 3D cross-linked graphene-based supercapacitors is one of the most urgent challenges for developing high-power energy supplies. We facilely synthesized a simple, eco-friendly, cost-effective heteroatoms (nitrogen, phosphorus, and fluorine) co-doped graphene oxide (NPFG) reduced by hydrothermal functionalization and freeze-drying approach with high specific surface areas and hierarchical pore structures. The effect of different heteroatoms doping on the energy storage performance of the synthesized reduced graphene oxide is investigated extensively. The electrochemical analysis performed in a three-electrode system via cyclic voltammetry (CV), galvanostatic charging-discharging (GCD), and electrochemical impedance spectroscopy (EIS) demonstrates that the nitrogen, phosphorous, and fluorine co-doped graphene (NPFG-0.3) synthesized with the optimum amount of pentafluoropyridine and phytic acid (PA) exhibits a notably enhanced specific capacitance (319 F g-1 at 0.5 A g-1), good rate capability, short relaxation time constant (τ = 28.4 ms), and higher diffusion coefficient of electrolytic cations (Dk+ = 8.8261 × 10-9 cm2 s-1) in 6 M KOH aqueous electrolyte. The density functional theory (DFT) calculation result indicates that the N, F, and P atomic replacement within the rGO model could increase the energy value (G T) from -673.79 eV to -643.26 eV, demonstrating how the atomic level energy could improve the electrochemical reactivity with the electrolyte. The improved performance of NPFG-0.3 over NFG, PG, and pure rGO is mainly ascribed to the fast-kinetic process owing to the well-balanced electron/ion transport phenomenon. A symmetric coin cell supercapacitor device fabricated using NPFG-0.3 as the anode and cathode material with 6 M KOH aqueous electrolyte exhibits maximum specific energy of 38 W h kg-1, a maximum specific power of 716 W kg-1, and ∼88.2% capacitance retention after 10 000 cycles. The facile synthesis approach and promising electrochemical results suggest this synthesized NPFG-0.3 material has high potential for future supercapacitor application.

Neutral oxygen irradiation enhanced forming-less ZnO-based transparent analog memristor devices for neuromorphic computing applications.

Surface oxidation employing neutral oxygen irradiation significantly improves the switching and synaptic performance of ZnO-based transparent memristor devices. The endurance of the as-irradiated device is increased by 100 times, and the operating current can be lowered by 10 times as compared with the as-deposited device. Moreover, the performance-enhanced device has an excellent analog behavior that can exhibit 3 bits per cell nonvolatile multistate characteristics and perform 15 stable epochs of synaptic operations with highly linear weight updates. A simulated artificial neural network comprising 1600 synapses confirms the superiority of the enhanced device in processing a 40 × 40 pixels grayscale image. The irradiation effectively decreases the concentration of oxygen vacancy donor defects and promotes oxygen interstitial acceptor defects on the surface of the ZnO films, which consequently modulate the redox process during rupture and rejuvenation of the filament. This work not only proposes the potential of ZnO-based memristor devices for high-density invisible data storage and in-memory computing application but also offers valuable insight in designing high-performance memristor devices, regardless of the oxide system used, by taking advantage of our neutral oxygen irradiation technique.

Role of precursors mixing sequence on the properties of CoMn2O4 cathode materials and their application in pseudocapacitor.

In this study, the effect of oxygen vacancy in the CoMn2O4 on pseudocapacitive characteristics was examined, and two tetragonal CoMn2O4 spinel compounds with different oxygen vacancy concentrations and morphologies were synthesized by controlling the mixing sequence of the Co and Mn precursors. The mixing sequence was changed; thus, morphologies were changed from spherical nanoparticles to nanoflakes and oxygen vacancies were increased. Electrochemical studies have revealed that tetragonal CoMn2O4 spinels with a higher number of oxygen vacancies exhibit a higher specific capacitance of 1709 F g-1 than those with a lower number of oxygen vacancies, which have a higher specific capacitance of 990 F g-1. Oxygen vacancies create an active site for oxygen ion intercalation. Therefore, oxidation-reduction reactions occur because of the diffusion of oxygen ions at octahedral/tetrahedral crystal edges. The solid-state asymmetric pseudocapacitor exhibits a maximum energy density of 32 Wh-kg-1 and an excellent cyclic stability of nearly 100%.

Synthesis of Free-Standing Flexible rGO/MWCNT Films for Symmetric Supercapacitor Application.

Herein, we report a novel, simple, and cost-effective way to synthesize flexible and conductive rGO and rGO/MWCNT freestanding films. The effects of MWCNT addition on the electrochemical performance of rGO/MWCNT nanocomposite films are investigated in some strong base aqueous electrolytes, such as KOH, LiOH, and NaOH via three-electrode system. The supercapacitor behavior of the films is probed via cyclic voltammetry, galvanostatic charging-discharging, and electrochemical impedance spectroscopy. The structural and morphological studies of the films are performed by X-ray diffractometer, Raman spectrometer, surface area analyzer, thermogravimetric analysis, field emission scanning electron microscope and transmission electron microscope. The rGO/MWCNT film synthesized with 10 wt% MWCNTs (GP10C) exhibits high specific capacitance of 200 Fg-1, excellent cyclic stability with 92% retention after 15,000 long cycle test, small relaxation time constant (~ 194 ms), and high diffusion coefficient (7.8457 × 10-9 cm2 s-1) in 2 M KOH electrolyte. Furthermore, the symmetric supercapacitor coin cell with GP10C as both anode and cathode using 2 M KOH as electrolyte demonstrates high energy density of 29.4 Whkg-1 and power density of 439 Wkg-1 at current density 0.1 Ag-1 and good cyclic stability with 85% retention of the initial capacitance at 0.3 Ag-1 after 10,000 cycles. Such a high performance of the GP10C film in the supercapacitor can be ascribed to the large surface area and small hydration sphere radius and high ionic conductivity of K+ cations in KOH electrolyte.

Improving linearity by introducing Al in HfO2 as a memristor synapse device.

Artificial synapse having good linearity is crucial to achieve an efficient learning process in neuromorphic computing. It is found that the synaptic linearity can be enhanced by engineering the doping region across the switching layer. The nonlinearity of potentiation and depression of the pure device is 36% and 91%, respectively; meanwhile, the nonlinearity after doping can be suppressed to be 22% (potentiation) and 60% (depression). Henceforth, the learning accuracy of the doped device is 91% with only 13 iterations; meanwhile, the pure device is 78%. A detailed conduction mechanism to understand this phenomenon is proposed.