Top Electrode Research Articles

Role of sulphur in resistive switching behavior of natural rubber-based memory

The rising environmental awareness has spurred the extensive use of green materials in electronic applications, with bio-organic materials emerging as attractive alternatives to inorganic and organic materials due to their natural biocompatibility, biodegradability, and eco-friendliness. This study showcases the natural rubber based resistive switching memory devices and how varying sulphur concentrations (0 - 0.8 wt.%) in natural rubber thin films impact the resistive switching characteristics. The natural rubber was formulated and processed into a thin film deposited on an ITO substrate as the bottom electrode and with an Ag film as the top electrode. The addition of sulphur modifies the degree of crosslinking in the natural rubber thin film, from which the concentration of -C=C- group and density of defect site (S+) are affected, and hence the resistive switching behavior of the memory device. The devices exhibit bipolar resistance with symmetric switching characteristics which are attributed to the formation of conductive paths facilitate by electron transport along -C=C- and S+ defect sites between the two electrodes. Notably, a sample with 0.2 wt.% sulphur exhibits a high ON/OFF ratio (104), a large memory window (5.5 V), prolonged data retention (10 years), and reliable endurance (120 cycles). These findings highlight the potential of natural rubber as a promising material for eco-friendly resistive-switching random access memory applications.&#xD.

Developing Screen-Printing Processes for Silver Electrodes Towards All-Solution Coating Processes for Solar Cells

In recent years, third-generation solar cells have experienced a remarkable growth in efficiency, making them a highly promising alternative energy solution. Currently, high-efficiency solar cells often use top electrodes fabricated by thermal evaporation, which rely on high-cost and high energy-consumption vacuum equipment, raising significant concerns for mass production. This study develops a method for fabricating silver electrodes using the screen-printing process, aiming to achieve solar cell production through an all-solution coating process. By selecting appropriate blocking-layer materials and optimizing the process, we have achieved device efficiencies for organic photovoltaics (OPVs) with screen-printed silver electrodes comparable to those with silver electrodes fabricated by thermal evaporation. Furthermore, we developed a method to cure the silver ink using near-infrared (NIR) annealing, significantly reducing the curing time from 30 min with hot air annealing to just 5 s. Additionally, by employing sheet-to-sheet (S2S) slot-die coating, we scaled up the device area and completed module development, successfully verifying stability in ambient air. We have also extended the application of screen-printed silver electrodes to perovskite solar cells (PSCs).

Resistive Switching Characteristics of NiO Thin Films Influenced by Changes in the Diameter of Nanometer-Scale Top Electrodes.

We investigated the forming, set, and reset voltages affected by the area of the top electrodes of a resistive random access memory (RRAM) capacitor fabricated by epitaxial NiO thin films. NiO RRAM capacitors with Au top electrode with a diameter of 100 μm showed typical unipolar switching characteristics. Au top electrodes with diameters of 10, 20, and 30 nm were formed on the surface of epitaxial NiO thin films by e-beam lithography. The forming, set, and reset voltages tended to decrease as the diameter of NiO RRAM capacitors with nanosized Au top electrodes decreased. As the area of the Au top electrodes increases, the volume of space in which the conductive filaments formed within the NiO RRAM capacitors can be formed becomes larger. This causes the conductive filament to be formed at relatively low energy, giving low forming voltages, while increasing the diversity of paths, causing a wide forming voltage distribution.

Investigation of Internal Thermal Distribution in Inverted Perovskite Solar Cell and Improvement of its Heat Dissipation Performance

Abstract COMSOL Multiphysics software was used to construct a numerical opto-electro-thermal coupling model to investigate the mechanisms of internal heat generation, conduction, and dissipation in inverted (p-i-n architecture) perovskite solar cells (PSCs). The research results indicate that Joule heating and Shockley-Read-Hall (SRH) recombination are the primary sources of heat, leading to significant accumulation of heat at the interfaces between the perovskite and the electron transport layer (ETL), as well as between the ETL and the electrode. This concentration of heat not only affects the performance of the device but also poses challenges for overall thermal management. Therefore, we compared four different top electrode materials (Ag, Cu, Al, and reduced graphene oxide) to assess their performance in terms of heat dissipation efficiency. The results showed that reduced graphene oxide (RGO) performed exceptionally well in heat dissipation efficiency, primarily due to its high thermal conductivity, which enables it to effectively reduce heat accumulation at the interfaces, thereby improving performance of PSCs. This finding provides important material selection criteria for optimizing the thermal management of PSCs.

In Situ IR Spectroscopy Studies of Atomic Layer-Deposited SnO2 on Fullerenes for Perovskite Photovoltaics.

In recent years, atomic layer deposition (ALD) has established itself as the state-of-the-art technique for the deposition of SnO2 buffer layers grown between the fullerene electron transport layer (ETL) and the ITO top electrode in metal halide perovskite-based photovoltaics. The SnO2 layer shields the underlying layers, i.e., the fullerene-derivative materials such as C60 and PCBM, as well as the perovskite absorber, from water ingress and damage induced by the sputtering of the transparent front contact. Our study undertakes a comprehensive investigation of the impact of SnO2 ALD processing on fullerenes by means of in situ spectroscopic ellipsometry (SE) and transmission infrared spectroscopy (FTIR). While no difference in SnO2 bulk properties is observed and the perovskite absorber degradation is nearly entirely avoided during exposure to heat and vacuum, when the absorber is introduced beneath the organic ETLs, a SnO2 growth delay of about 50 ALD cycles is measured on PCBM, whereas the delay is limited to 10 cycles in the case of growth on C60. Notably, FTIR measurements show that while C60 remains chemically unaffected during SnO2 ALD growth, PCBM undergoes chemical modification, specifically of its ester groups. The onset of these modifications corresponds with the detection of the onset, after the initial delay, of ALD SnO2 growth. It is expected that the modification that the PCBM layer undergoes upon ALD SnO2 processing is responsible for the systematic lower photovoltaic device performance in the case of PCBM-based devices, with respect to C60-based devices.

A multilevel resistive switching memristor based on flexible organic–inorganic hybrid film with recognition function

Abstract Brain-inspired neuromorphic computing systems fueled the emergence of memristor-based artificial synapses, however, conventional silicon-based devices restricted their usage in the wearable field because of their difficulty in bending. To tackle the above challenge, a vertically structured flexible memristor with aluminum-based hydroquinone organic–inorganic hybrid film and Al2O3 as the functional layer, ITO and Pt as the bottom and top electrodes, and PET as the substrate has been developed utilizing molecular/atomic layer deposition to achieve a tradeoff between the resistive transition properties and the flexibility of memristors. The obtained devices combine stable resistive switching behavior and flexibility, showing high switching ratio of 103, better retention (up to 105 s) and endurance properties (up to 104 cycles), and robustness at radius of curvature of 4.5 mm after 104 bending cycles. Furthermore, the presence of multilevel resistive states in these devices ensures that the memristor can emulate synaptic properties such as paired-pulse facilitation, transition from short-term plasticity to long-term plasticity, long-term potentiation and depression, and spike-time-dependent plasticity. The resistive switching mechanism and the role of the bending state on the electrical performance of the device are explored. The fully connected artificial neural network based on the memristor can achieve a recognition accuracy of 90.2% for handwritten digits after training and learning. Flexible memristor will bring feasible advances to the integration of neuromorphic computing and wearable functionality.

Multistate Ferroelectric Diodes with High Electroresistance Based on van der Waals Heterostructures.

Some van der Waals (vdW) materials exhibit ferroelectricity, making them promising for novel nonvolatile memories (NVMs) such as ferroelectric diodes (FeDs). CuInP2S6 (CIPS) is a well-known vdW ferroelectric that has been integrated with graphene for memory devices. Here we demonstrate FeDs with self-rectifying, hysteretic current-voltage characteristics based on vertical heterostructures of 10 nm thick CIPS and graphene. By using vdW indium-cobalt top electrodes and graphene bottom electrodes, we achieve a high electroresistance (on- and off-state resistance ratios) of ∼106, an on-state rectification ratio of 2500 for read/write voltages of 2 V/0.5 V, and a maximum output current density of 100 A/cm2. These metrics compare favorably with state-of-the-art FeDs. Piezoresponse force microscopy measurements show that stabilization of intermediate net polarization states in CIPS leads to stable multibit data retention at room temperature. The combination of two-terminal design, multibit memory, and low-power operation in CIPS-based FeDs is potentially interesting for compute-in-memory and neuromorphic computing applications.

The role of flow field dynamics in enhancing volatile organic compound conversion in a surface dielectric barrier discharge system

Abstract This study investigates the correlation between flow fields induced by a surface dielectric barrier discharge (SDBD) system and its application for the volatile organic compound (VOC) gas conversion process. As a benchmark molecule, the conversion of n-butane is monitored using flame ionization detectors, while the flow field is analysed using planar particle image velocimetry. Two individual setups are developed to facilitate both conversion measurement and investigation of induced fluid dynamics. Varying the gap distance between two SDBD electrode plates for three different n-butane mole fractions reveals local peaks in relative conversion around gap distances of 16 mm to 22 mm, indicating additional spatially dependent effects. The lowest n-butane mole fractions exhibit the highest relative conversion, while the highest n-butane mole fraction conversion yields the greatest number of converted molecules per unit time. Despite maintaining constant energy density, the relative conversion exhibits a gradual decrease with increasing distances. The results of the induced flow fields reveal distinct vortex structures at the top and bottom electrodes, which evolve in size and shape as the gap distances increase. These vortices exhibit gas velocity magnitudes approximately seven times higher than the applied external gas flow velocity. Vorticity and turbulent kinetic energy analyses provide insights into these structures' characteristics and their impact on gas mixing. A comparison of line profiles through the centre of the vortices shows peaks in the middle gap region for the same gap distances, correlating with the observed peaks in conversion. These findings demonstrate a correlation between induced flow dynamics and the gas conversion process, bridging plasma actuator studies with the domain of chemical plasma gas conversion.

Enhanced analog switching and neuromorphic performance of ZnO-based memristors with indium tin oxide electrodes for high-accuracy pattern recognition.

This study systematically investigates analog switching and neuromorphic characteristics in a ZnO-based memristor by varying the anodic top electrode (TE) materials [indium tin oxide (ITO), Ti, and Ta]. Compared with the TE materials (Ti and Ta), memristive devices with TEs made of ITO exhibit dual volatile and nonvolatile switching behavior and multistate switching characteristics assessed based on reset-stop voltage and current compliance (ICC) responses. The polycrystalline structure of the ZnO functional layer sandwiched between ITO electrodes was confirmed by high-resolution transmission electron microscopy analysis. The current transport mechanism in the ZnO-based memristor was dominated by Schottky emission, with the Schottky barrier height modulated from 0.26 to 0.4V by varying the reset-stop voltage under different ICC conditions. The long-term potentiation and long-term depression synaptic characteristics were successfully mimicked by modulating the pulse amplitudes. Furthermore, a 90.84% accuracy was achieved using a convolutional neural network architecture for Modified National Institute of Standards and Technology pattern categorization, as demonstrated by the confusion matrix. The results demonstrated that the ITO/ZnO/ITO/Si memristor device holds promise for high-performance electronic applications and effective ITO electrode modeling.

Effect of SiCN thin film interlayer for ZnO-based RRAM.

This study investigates the effect of silicon carbon nitride (SiCN) as an interlayer for ZnO-based resistive random access memory (RRAM). SiCN was deposited using plasma-enhanced chemical vapor deposition (PECVD) with controlled carbon content, achieved by varying the partial pressure of tetramethylsilane (4MS). Our results indicate that increasing the carbon concentration enhances the endurance of RRAM devices but reduces the on/off ratio. Devices with SiCN exhibited lower operating voltages and more uniform resistive switching behavior. Oxygen migration from ZnO to SiCN is examined by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses, promoting the formation of conductive filaments (CFs) and lowering set voltages. Additionally, we examined the impact of top electrode oxidation on RRAM performance. The oxidation of the Ti top electrode was found to reduce endurance and increase low resistive state (LRS) resistance, potentially leading to device failure through the formation of an insulating layer between the electrode and resistive switching material. The oxygen storage capability of SiCN was further confirmed through high-temperature stress tests, demonstrating its potential as an oxygen reservoir. Devices with a 20 nm SiCN interlayer showed significantly improved endurance, with over 500 switching cycles, compared to 62 cycles in those with a 5 nm SiCN layer. However, the thicker SiCN layer resulted in a notably lower on/off ratio due to reduced capacitance. These findings suggest that SiCN interlayers can effectively enhance the performance and endurance of ZnO-based RRAM devices by acting as an oxygen reservoir and mitigating the top electrode oxidation effect.

Mitigating interfacial recombination enabling efficient semitransparent organic photovoltaics

Charge recombination at the interface between top electrode and active layer is a substantial current loss pathway in semitransparent organic photovoltaics (STOPVs). Reducing interfacial traps is an effective strategy to mitigate interfacial recombination and promote charge extraction, and thereby improve the power conversion efficiencies (PCEs). Herein, a facile approach of depositing 11-mercapto-undecanoic acid (11-MUA) on zinc oxide (ZnO) cathode interlayer in conventional STOPVs is demonstrated. 11-MUA can form covalent interactions with both ZnO and silver (Ag) and thus can induce the formation of high-quality ultrathin Ag electrode. Compared with that deposited on bare ZnO, the Ag electrode on ZnO/11-MUA shows higher conductivity as well as higher optical transparency. The STOPVs based on ZnO/11-MUA/Ag exhibit 2 orders of magnitude lower surface trap density than the counterparts based on ZnO/Ag. Consequently, 11-MUA simultaneously improves the PCEs from 11.2% to 12.1% and average visible transmittance from 21.6% to 27.0% in the STOPVs. Furthermore, arising from the 11-MUA-modified interface, the thermal stability of STOPVs based on ZnO/11-MUA/Ag is also improved.

Impact Deposition of a Single Droplet of Low-Melting-Point Alloy as the Top Electrode for Organic Photovoltaics.

Top electrodes of organic photovoltaics (OPVs) are usually thermally evaporated in the vacuum, which is non-continuous and time-consuming and has been the bottleneck for the OPV fabrication process. Printable top electrodes that are free of vacuum, high temperature, and solvents will make OPVs more attractive. Low-melting-point alloys (LMPAs) are promising candidates for printable OPV electrodes thanks to the merits of matching work functions, high electron conductivity, high environment stability, and no need for post-treatment. Here, LMPA electrodes are directly deposited on OPVs by simply falling a single LMPA droplet onto the substrate. The LMPA droplet spreads to form a thin film with a smooth interface intimately contacting the substrate. The electrode area can be tailored by adjusting the droplet diameter or the Weber number, which is the ratio of inertia to surface tension. The interface morphology is mainly affected by the contact temperature. The degree of oxidation and charges on the droplet can also influence the electrode area and interface morphology. OPVs with droplet-impacted LMPA electrodes exhibit power conversion efficiencies of up to 16.17%. This work demonstrates the potential of single-droplet impact deposition as a simple method for printing OPV electrodes for scalable manufacturing.

Nanoscale grating-based perovskite solar cell with improved efficiency

MAPbI3 perovskite-based solar cell (PSC) has attracted much attention due to its high absorption rate. The top flat electrode degrades the behavior of PSC due to limiting the light reached to the absorber layer, which reduces the efficiency. In this study, the influence of texturing the top FTO electrode surface with a triangular saw-tooth grating on both the optical and electrical performance is reported. The interference effects are also considered in this work by modeling the PSC structure as a Fabry–Perot resonator. In this regard, the finite difference time domain method is utilized to precisely simulate the optical characteristics of the nano-structural design. Also, the optical behavior of PSC is studied at different triangular grating (TG) structures and dimensions at which the light absorption is maximized. Furthermore, the effect of absorber thickness and defect density on the optoelectronic performance is investigated. We configured the conversion efficiency (η) of the proposed PSC structure by using the bulk and Langevin recombination mechanisms. The proposed grating structure enhances the light coupling, and hence the light absorption and the generated current density are increased. For absorber thickness of 350 nm, we reported a maximum conversion efficiency (η) of 19.5% for the proposed triangular grating (TG) structure with an enhancement of 19.6% compared to the structure with a flat FTO layer. As the defect density is increased from 1012 cm−3 to 1018 cm−3, the efficiency of the optimum TG PSC is reduced from 19.5% to 10.1%, respectively. The simulation results, therefore, contribute to the understanding of the PSC-based MAPbI3 design and can be used to improve its physical behavior.

GeTe/MoTe2 Van der Waals Heterostructures: Enabling Ultralow Voltage Memristors for Nonvolatile Memory and Neuromorphic Computing Applications.

Advanced electronic semiconducting Van der Waals heterostructures (HSs) are promising candidates for exploring next-generation nanoelectronics owing to their exceptional electronic properties, which present the possibility of extending their functionalities to diverse potential applications. In this study, GeTe/MoTe2 HS are explored for nonvolatile memory and neuromorphic-computing applications. Sputter-deposited Ag/GeTe/MoTe2/Pt HS cross-point devices are fabricated, and they demonstrate memristor behavior at ultralow switching voltages (VSET: 0.15V and VRESET: -0.14V) with very low energy consumption (≈30 nJ), high memory window, long retention time (104 s), and excellent endurance (105 cycles). Resistive switching is achieved by adjusting the interface between the Ag top electrode and the heterojunction switching layer. Cross-sectional transmission electron microscope images and conductive atomic force microscopy analysis confirm the presence of a conducting filament in the heterojunction switching layer. Further, emulating various synaptic functions of a biological synapse reveals that GeTe/MoTe2 HS can be utilized for energy-efficient neuromorphic-computing applications. A multilayer perceptron is implemented using the synaptic weights of the Ag/GeTe/MoTe2/Pt HS device, revealing high pattern accuracy (81.3%). These results indicate that HS devices can be considered a potential solution for high-density memory and artificial intelligence applications.

3D Optical Wedge and Movable Optical Axis LC Lens

Current liquid crystal (LC) lenses cannot achieve lossless arbitrary movement of the optical axis without mechanical movement. This article designs a novel bottom electrode through simulation and optimization, which forms a special LC lens with an Archimedean spiral electrode, realizing a 3D LC wedge and an arbitrarily movable LC lens. When only the bottom electrode is controlled, it achieves a maximum beam steering angle of 0.164°, which is nearly an order of magnitude larger than the current design. When the top and bottom electrodes are controlled jointly, a 0.164° movement of the lens optical axis is achieved. With focal length varies, the movement of the optical axis ranges from zero to infinity, and the lens surface remains unchanged during movement. The focus can move in a 3D conical area. When the thickness of the LC layer is 30 μm, the fastest response time reaches only 0.635 s, much faster than now.

High-Performance Red Transparent Quantum Dot Light-Emitting Diodes via Fully Solution-Processed MXene/Ag NWs Top Electrode.

The integration of high-performance transparent top electrodes with the functional layers of transparent quantum dot light-emitting diodes (T-QLEDs) poses a notable challenge. This study presents a composite transparent top electrode composed of MXene and Ag NWs. The composite electrode demonstrates exceptional transparency (84.6% at 620 nm) and low sheet resistance (16.07 Ω sq-1), rendering it suitable for integration into T-QLEDs. The inclusion of MXene nanosheets in the composite electrode serves a dual role: adjusting the work function to enhance electron injection efficiency and enhancing the interface between Ag NWs and the emissive layer, thereby mitigating the common issue of interfacial resistance in conventional transparent electrodes. This strategic amalgamation results in notable improvements in device performance, yielding a maximum current efficiency of 23.12 cd A-1, an external quantum efficiency of 13.98%, and a brightness of 21,015 cd m-2. These performance metrics surpass those achieved by T-LEDs employing pristine Ag NW electrodes. This study offers valuable insights into T-QLED device advancement and provides a promising approach for transparent electrode fabrication in optoelectronic applications.

Thermally Triggered Interface for Simplified Organic Solar Cells

Organic photovoltaic (OPV) cells are commonly produced by successive printing of four layers on top of a transparent conducting electrode, with the active layer sandwiched in between interlayers followed by the top electrode. Here, the simplification of OPV manufacturing without the need to coat a hole transport layer (HTL) in inverted OPV (n–i–p) is reported. To ensure the required hole selectivity, thermally trigged molecules are directly blended in the active layer during device casting. Following thermal annealing of the complete devices, organosulfur molecules self‐assembled to form a hole–transporting interface between the silver top electrode and the active layer, thereby enabling working devices. Device optimization is performed by varying the concentration of these molecules and the thermal annealing conditions. The performances of the simplified devices approach those of control devices with vacuum‐evaporated MoO3 HTLs. The solar cells exhibit very encouraging thermal and photostabilities. This work opens the route to high efficiency, simplified, and low‐cost organic solar cells.

Flexible Crossbar Molecular Devices with Patterned EGaIn Top Electrodes for Integrated All-Molecule-Circuit Implementation.

Here, a unique crossbar architecture is designed and fabricated, incorporating vertically integrated self-assembled monolayers in electronic devices. This architecture is used to showcase 100 individual vertical molecular junctions on a single chip with a high yield of working junctions and high device uniformity. The study introduces a transfer approach for patterned liquid-metal eutectic alloy of gallium and indium top electrodes, enabling the creation of fully flexible molecular devices with electrical functionalities. The devices exhibit excellent charge transport performance, sustain a high rectification ratio (>103), and stable endurance and retention properties, even when the devices are significantly bent. Furthermore, Boolean logic gates, including OR and AND gates, as well as half-wave and full-wave rectifying circuits, are successfully implemented. The unique design of the flexible molecular device represents a significant step in harnessing the potential of molecular devices for high-density integration and possible molecule-based computing.

Data encryption/decryption and medical image reconstruction based on a sustainable biomemristor designed logic gate circuit

Memristors are considered one of the most promising new-generation memory technologies due to their high integration density, fast read/write speeds, and ultra-low power consumption. Natural biomaterials have attracted interest in integrated circuits and electronics because of their environmental friendliness, sustainability, low cost, and excellent biocompatibility. In this study, a sustainable biomemristor with Ag/mugwort:PVDF/ITO structure was prepared using spin-coating and magnetron sputtering methods, which exhibited excellent durability, significant resistance switching (RS) behavior and unidirectional conduction properties when three metals were used as top electrode. By studying the conductivity mechanism of the device, a charge conduction model was established by the combination of F-N tunneling, redox, and complexation reaction. Finally, the novel logic gate circuits were constructed using the as-prepared memristor, and further memristor based encryption circuit using 3-8 decoder was innovatively designed, which can realize uniform rule encryption and decryption of medical information for data and medical images. Therefore, this work realizes the integration of memristor with traditional electronic technology and expands the applications of sustainable biomemristors in digital circuits, data encryption, and medical image security.

Diffusive Memristor with CuS Nanoparticles Embedded in Polymeric Film as Artificial Nociceptor.

The threshold behavior and the ion diffusion dynamics in diffusive volatile memristors have a very uncanny resemblance to the transduction process of biological nociceptors. Hence, the diffusive memristors are considered the most suited for making artificial nociceptive systems. To facilitate their widespread adoption, it is imperative to develop polymeric or organic-inorganic hybrid material-based diffusive memristors that are economical, biocompatible, and easily processable. In this study, we present a cluster-type polymeric diffusive memristor where copper is used as the active top electrode. The switching medium comprises copper(II) sulfide (CuS) nanoparticles embedded in poly(ethylene oxide) (PEO). The devices show electrochemical metalization (ECM)-type and bidirectional diffusive volatile memory with high nonlinearity (104) and turn-on slope (5.6 mV/dec). They reliably remain diffusive volatile with up to 10 wt % CuS in PEO and for a wide range of compliance (10-6 to 10-2 A) without transitioning to the bipolar nonvolatile type. The low reduction potential of CuS and optimal segmental dynamics of PEO work synergistically to ensure stable and reproducible diffusive memory. The CuS nanoparticles act as bipolar electrodes, undergoing local oxidation and reduction under the influence of the bias. The switching of resistance states in the CuS-PEO memristors is attributed to the formation of cluster-type filaments between CuS nanoparticles within the PEO matrix supported by the participation of copper ions from the top Cu electrode. The observation of low filament temperature and the independence of on-state resistance with respect to the device area and temperature further corroborate the cluster-type filament in CuS-PEO memristors. Using a 5 wt % CuS-based device, an artificial nociceptor is realized, which successfully mimics most of the nociceptive plasticities such as threshold, relaxation, no adaptation, and sensitization.