Pushing the conductance and transparency limit of monolayer graphene electrodes for flexible organic light-emitting diodes.

Graphene has emerged as an attractive candidate for flexible transparent electrode (FTE) for a new generation of flexible optoelectronics. Despite tremendous potential and broad earlier interest, the promise of graphene FTE has been plagued by the intrinsic trade-off between electrical conductance and transparency with a figure of merit (σDC/σOp) considerably lower than that of the state-of-the-art ITO electrodes (σDC/σOp <123 for graphene vs. ∼240 for ITO). Here we report a synergistic electrical/optical modulation strategy to simultaneously boost the conductance and transparency. We show that a tetrakis(pentafluorophenyl)boric acid (HTB) coating can function as highly effective hole doping layer to increase the conductance of monolayer graphene by sevenfold and at the same time as an anti-reflective layer to boost the visible transmittance to 98.8%. Such simultaneous improvement in conductance and transparency breaks previous limit in graphene FTEs and yields an unprecedented figure of merit (σDC/σOp ∼323) that rivals the best commercial ITO electrode. Using the tailored monolayer graphene as the flexible anode, we further demonstrate high-performance green organic light-emitting diodes (OLEDs) with the maximum current, power and external quantum efficiencies (111.4 cd A-1, 124.9 lm W-1 and 29.7%) outperforming all comparable flexible OLEDs and surpassing that with standard rigid ITO by 43%. This study defines a straightforward pathway to tailor optoelectronic properties of monolayer graphene and to fully capture their potential as a generational FTE for flexible optoelectronics.

Testing the Uniformity of Surface Resistance on Large-Format Transparent Heating Glass.

The design of a glazing package containing heating glass can make a window a radiator simultaneously. For such bulky glass to act as an effective radiator simultaneously, it should be possible to provide a constant temperature over the entire surface. The continuous surface temperature of the glass depends on the uniformity of the surface resistance of the resistive layer. This paper will demonstrate the testing of heating glass parameters using a specialised apparatus. The research will mainly focus on measuring the value and distribution of the surface resistance of the transparent heating layer. A thermographic study will verify the results. As the heating glass will be subjected to a toughening process, the effect of the toughening process parameters on the degradation of the transparent heating film will be investigated.

WSe2 as Transparent Top Gate for Infrared Near-Field Microscopy.

Independent control of carrier density and out-of-plane displacement field is essential for accessing novel phenomena in two-dimensional (2D) material heterostructures. While this is achieved with independent top and bottom metallic gate electrodes in transport experiments, it remains a challenge for near-field optical studies as the top electrode interferes with the optical path. Here, we characterize the requirements for a material to be used as the top-gate electrode and demonstrate experimentally that few-layer WSe2 can be used as a transparent, ambipolar top-gate electrode in infrared near-field microscopy. We carry out nanoimaging of plasmons in a bilayer graphene heterostructure tuning the plasmon wavelength using a trilayer WSe2 gate, achieving a density modulation amplitude exceeding 2 × 1012 cm-2. The observed ambipolar gate-voltage response allows us to extract the energy gap of WSe2, yielding a value of 1.05 eV. Our results provide an additional tuning knob to cryogenic near-field experiments on emerging phenomena in 2D materials and moiré heterostructures.

Room-temperature nanojoining of silver nanowires by graphene oxide for highly conductive flexible transparent electrodes.

Flexible transparent electrodes for touch panels, solar cells, and wearable electronics are in great demand in recent years, and the silver nanowire (AgNW) flexible transparent electrode (FTE) is among the top candidates due to its excellent light transmittance and flexibility and the highest conductivity of silver among all metals. However, the conductivity of an AgNWs network has long been limited by the large contact resistance. Here we show a room-temperature solution process to tackle the challenge by nanojoining AgNWs with two-dimensional graphene oxide (GO). The conductivity of the AgNWs network is improved 18 times due to the enhanced junctions between AgNWs by the coated GOs, and the AgNW-GO FTE exhibits a low sheet resistance of 23 Ohm sq-1and 88% light transmittance. It is stable under high temperature and current and their flexibility is intact after 1000 cycles of bending. Measurements of a bifunctional electrochromic device shows the high performance of the AgNW-GO FTE as a FTE.

Highly stable semitransparent multilayer graphene/LaVO3vertical-heterostructure photodetectors.

A heterostructure composed of a combination of semi-metallic graphene (Gr) and high-absorption LaVO3is ideal for high-performance translucent photodetector (PD) applications. Here, we present multilayer Gr/LaVO3vertical-heterostructure semitransparent PDs with various layer numbers (Ln). AtLn= 2, the PD shows the best performance with a responsivity (R) of 0.094 A W-1and a specific detectivity (D*) of 7.385 × 107cm Hz1/2W-1at 532 nm. Additionally, the average visible transmittance of the PD is 63%, i.e. it is semitransparent. We increased photocurrent (PC) by approximately 13%, from 0.564 to 0.635µA cm-2by using an Al reflector on the semitransparent PD. The PC of an unencapsulated PD maintains about 86% (from 0.571 to 0.493µA cm-2) of its initial PC value after 2000 h at 25 °C temperature/30% relative humidity, showing good stability. This behavior is superior to that of previously reported graphene-based PDs. These results show that these PDs have great potential for semitransparent optoelectronic applications.

A solvent-compatible filter-transfer method of semi-transparent carbon-nanotube electrodes stacked with silver nanowires.

Low-density films of single-walled carbon nanotubes (SWNTs) can be used as a semi-transparent top electrode for all-solution-processed film devices; however, their semiconductor characteristics vary depending on the experimental factors in their dispersion into solvents, and the sublayers are damaged as a result of solvent incompatibility. In this study, we report a solvent-compatible filter-transfer method for SWNT films stacked with silver nanowires (AgNWs), and evaluate the semiconductor characteristics through the p/n heterojunction with a Si wafer (SWNT/Si). AgNWs and SWNTs were successively filtered through their aqueous dispersion solutions using a membrane filter. The stacked semi-transparent films (AgNW/SWNT films with controlled densities) were successfully transferred onto glass plates and Si wafers. The transmittance at 550 nm revealed a window between 60% and 80% with a narrow sheet resistance range between 11 and 23 Ω â–¡-1. The power conversion efficiency (PCE) of SWNT/Si was improved to 11.2% in a junction area of 0.031 cm2 through the use of spin-coated Nafion resins; however, the accumulated resistance of SWNTs drastically reduced the PCE to 2% as the area increased to ≥0.5 cm2. AgNWs maintained the PCE within a range of 10.7% to 8.6% for an area ranging from 0.031 cm2 to 1.13 cm2. All of the photovoltaic parameters were dependent on the junction areas, suggesting that AgNWs function as an effective current-collector layer on the semiconductor layer of SWNTs without direct contact of AgNWs with the Si surface. In addition, we report a solvent-compatible experiment for transferring AgNW/SWNT films onto a solvent-sensitive perovskite material (CH3NH3PbI3).

Label-Free Probing of Electron Transfer Kinetics of Single Microbial Cells on a Single-Layer Graphene via Structural Color Microscopy.

Studies of electron transfer at the population level veil the nature of the cell itself; however, in situ probing of the electron transfer dynamics of individual cells is still challenging. Here we propose label-free structural color microscopy for this aim. We demonstrate that Shewanella oneidensis MR-1 cells show unique structural color scattering, changing with the redox state of cytochrome complexes in the outer membrane. It enables quantitatively and noninvasive studies of electron transfer in single microbial cells during bioelectrochemical activities, such as extracellular electron transfer (EET) on a transparent single-layer graphene electrode. Increasing the applied potential leads to the associated EET current, accompanied by more oxidized cytochromes. The high spatiotemporal resolution of the proposed method not only demonstrates the large diversity in EET activity among microbial cells but also reveals the subcellular asymmetric distribution of active cytochromes in a single cell. We anticipate that it provides a potential platform for further exploring the electron transfer mechanism of subcellular structure.

Optically transparent electrodes to study living cells: A mini review.

The use of electrochemical methods to study living systems, including cells, has been of interest to researchers for a long time. Thus, controlling the polarization of the electrode contacting living cells, one can influence, for example, their proliferation or the synthesis of specific proteins. Moreover, the electrochemical approach formed the basis of the biocompatibility improvement of the materials contacting with body tissues that use in carbon hemosorbents and implants development. It became possible to reach a fundamentally new level in the study of cell activity with the introduction of optically transparent electrodes in this area. The advantage of the using of optically transparent electrodes is the possibility of simultaneous analysis of living cells by electrochemical and microscopic methods. The use of such materials allowed approaching to the study of the influence of the electrode potential on adhesion activity and morphology of the different cell types (HeLa cells, endothelial cell, etc.) more detailed. There are a negligible number of publications in this area despite the advantages of the usage of optically transparent electrodes to study living cells. This mini-review is devoted to some aspects of the interaction of living cells with conductive materials and current advances in the use of optically transparent electrodes for the study of living cells, as well as the prospects for their use in cellular technologies.

Synthesis of transparent bio-electrodes for biophysiological measurements based on modified graphene oxide.

The main objective of this work was to fabricate smart nanocomposite transparent conductive biophysiological electrodes based on modified graphene oxide (GO). The GO is abundant, flexible conductors that can be formulated as a transparent sheet and thereby alleviate the drawbacks of using indium tin oxide in transparent electrodes, like its scarcity, brittleness, and cost. GO was synthesized by a modified version of Hummers' method under highly acidic conditions with sulfuric acid and showed good distribution at a high temperature of 90 °C. Polyvinyl alcohol (PVA) was used as a polymer host in the composite. Glycerol (Gl) was used to increase the flexibility and conductivity through an esterification reaction. Characteristic techniques were used to detect the morphology and structure of GO fillers and their polymer composites, such as transmission electron microscopy, x-ray diffraction, scanning electron microscopy and Fourier transform infrared spectroscopy. The GO/Gl/PVA transparent nanocomposite was tested for the synthesis of electrocardiogram (ECG) and electrodermal (EDA) electrodes. The Biopac device was used to evaluate the behavior of the GO/Gl/PVA plastic transparent electrode in comparison to the GO/Gl/PVA black electrode and a commercial one. The results indicated improved efficiency of the GO/Gl/PVA ECG transparent electrode. The GO/Gl/PVA EDA electrode produced signals with higher conductivity and lower noise than the commercial electrode.

Rapid nanowelding of silver nanowires by focused-light-scanning for high-performance flexible transparent electrodes.

Silver nanowires (AgNWs) have been considered as one of the most promising flexible transparent electrodes (FTEs) material for next-generation optoelectronic devices. However, the large contact resistance between AgNWs could deteriorate the conductivity of FTEs. In the present work, high-performance AgNWs FTEs were obtained by means of focused-light-scanning (FLS), which could lead to the large-area, rapid and high-quality welding between AgNWs within a short time, forming the reliable and stable AgNWs network. The results of the optoelectronic tests show that after FLS, the sheet resistance of the AgNWs FTEs sharply decreased from 5113 Ω/sq to 7.7 Ω/sq, with maintaining a high transmittance (∼94%). Finally, a high-performance flexible transparent heater was fabricated by using FLS, showing reach a relatively high temperature in a short response time and rapid response at low input voltage. The findings offer an effective pathway to greatly improve the conductivity of AgNWs FTEs.

High-performance flexible transparent micro-supercapacitors from nanocomposite electrodes encapsulated with solution processed MoS2 nanosheets.

Two-dimensional molybdenum disulfide (MoS2) nanosheets have emerged as a promising material for transparent, flexible micro-supercapacitors, but their use in electrodes is hindered by their poor electrical conductivity and cycling stability because of restacking. In this paper, we report a novel electrode architecture to exploit electrochemical activity of MoS2 nanosheets. Electrochemically exfoliated MoS2 dispersion was spin coated on mesh-like silver networks encapsulated with a flexible conducting film exhibiting a pseudocapacitive behavior. MoS2 nanosheets were electrochemically active over the whole electrode surface and the conductive layer provided a pathway to transport electrons between the MoS2 and the electrolyte. As the result, the composite electrode achieved a large areal capacitance (89.44 mF cm-2 at 6 mA cm-2) and high energy and power densities (12.42 µWh cm-2 and P = 6043 µW cm-2 at 6 mA cm-2) in a symmetric cell configuration with 3 M KOH solution while exhibiting a high optical transmittance of ~80%. Because the system was stable against mechanical bending and charge/discharge cycles, a flexible micro-supercapacitor that can power electronics at different bending states was realized.

Near-Field Electrospinning for Three-Dimensional Stacked Nanoarchitectures with High Aspect Ratios.

Near-field electrospinning (NFES) was developed to overcome the intrinsic instability of traditional electrospinning processes and to facilitate the controllable deposition of nanofibers under a reduced electric field. This technique offers a straightforward and versatile method for the precision patterning of two-dimensional (2D) nanofibers. However, three-dimensional (3D) stacked structures built by NFES have been limited to either micron-scale sizes or special shapes. Herein, we report on a direct-write 3D NFES technique to construct self-aligned, template-free, 3D stacked nanoarchitectures by simply adding salt to the polymer solution. Numerical simulations suggested that the electric field could be tuned to achieve self-aligned nanofibers by adjusting the conductivity of the polymer solution. This was confirmed experimentally by using poly(ethylene oxide) (PEO) solutions containing 0.1-1.0 wt% NaCl. Using 0.1 wt% NaCl, nanowalls with a maximum of 80 layers could be built with a width of 92 ± 3 nm, height of 6.6 ± 0.1 µm, and aspect ratio (height/width) of 72. We demonstrate the 3D printing of nanoskyscrapers with various designs, such as curved "nanowall arrays", nano "jungle gyms," and "nanobridges". Further, we present an application of the 3D stacked nanofiber arrays by preparing transparent and flexible polydimethylsiloxane films embedded with Ag-sputtered nanowalls as 3D nanoelectrodes. The conductivity of the nanoelectrodes can be precisely tuned by adjusting the number of 3D printed layers, without sacrificing transmittance (98.5%). The current NFES approach provides a simple, reliable route to build 3D stacked nanoarchitectures with high-aspect ratios for potential application in smart materials, energy devices, and biomedical applications.

Transparent, conformable, active multielectrode array using organic electrochemical transistors.

Mechanically flexible active multielectrode arrays (MEA) have been developed for local signal amplification and high spatial resolution. However, their opaqueness limited optical observation and light stimulation during use. Here, we show a transparent, ultraflexible, and active MEA, which consists of transparent organic electrochemical transistors (OECTs) and transparent Au grid wirings. The transparent OECT is made of Au grid electrodes and has shown comparable performance with OECTs with nontransparent electrodes/wirings. The transparent active MEA realizes the spatial mapping of electrocorticogram electrical signals from an optogenetic rat with 1-mm spacing and shows lower light artifacts than noise level. Our active MEA would open up the possibility of precise investigation of a neural network system with direct light stimulation.

Stretchable Transparent Electrode Arrays for Simultaneous Electrical and Optical Interrogation of Neural Circuits in Vivo.

Recent developments of transparent electrode arrays provide a unique capability for simultaneous optical and electrical interrogation of neural circuits in the brain. However, none of these electrode arrays possess the stretchability highly desired for interfacing with mechanically active neural systems, such as the brain under injury, the spinal cord, and the peripheral nervous system (PNS). Here, we report a stretchable transparent electrode array from carbon nanotube (CNT) web-like thin films that retains excellent electrochemical performance and broad-band optical transparency under stretching and is highly durable under cyclic stretching deformation. We show that the CNT electrodes record well-defined neuronal response signals with negligible light-induced artifacts from cortical surfaces under optogenetic stimulation. Simultaneous two-photon calcium imaging through the transparent CNT electrodes from cortical surfaces of GCaMP-expressing mice with epilepsy shows individual activated neurons in brain regions from which the concurrent electrical recording is taken, thus providing complementary cellular information in addition to the high-temporal-resolution electrical recording. Notably, the studies on rats show that the CNT electrodes remain operational during and after brain contusion that involves the rapid deformation of both the electrode array and brain tissue. This enables real-time, continuous electrophysiological monitoring of cortical activity under traumatic brain injury. These results highlight the potential application of the stretchable transparent CNT electrode arrays in combining electrical and optical modalities to study neural circuits, especially under mechanically active conditions, which could potentially provide important new insights into the local circuit dynamics of the spinal cord and PNS as well as the mechanism underlying traumatic injuries of the nervous system.

Pressure Welding of Silver Nanowires Networks at Room Temperature as Transparent Electrodes for Efficient Organic Light-Emitting Diodes.

In this work, polymethylmethacrylate (PMMA) as a superior mediate for the pressure welding of silver nanowires (Ag NWs) networks as transparent electrodes without any thermal treatment is demonstrated. After a pressing of 200 kg cm-2 , not only the sheet resistance but also the surface roughness of the PMMA-mediated Ag NWs networks decreases from 2.6 kΩ sq-1 to 34.3 Ω sq-1 and from 76.1 to 12.6 nm, respectively. On the other hand, high transparency of an average transmittance in the visible wavelengths of 93.5% together with a low haze value of 2.58% can be achieved. In terms of optoelectronic applications, the promising potential of the PMMA-mediated pressure-welded Ag NWs networks used as a transparent electrode in a green organic light-emitting diode (OLED) device is also demonstrated. In comparison with the OLED based on commercial tin-doped indium oxide electrode, the increments of power efficiency and external quantum efficiency (EQE) from 80.1 to 85.9 lm w-1 and 19.2% to 19.9% are demonstrated. In addition, the PMMA-mediated pressure welding succeeds in transferring Ag NWs networks to flexible polyethylene naphthalate and polyimide substrates with the sheet resistance of 42 and 91 Ω sq-1 after 10 000 times of bending, respectively.

Capillary-Force-Induced Cold Welding in Silver-Nanowire-Based Flexible Transparent Electrodes.

Silver nanowire (AgNW) films have been studied as the most promising flexible transparent electrodes for flexible photoelectronics. The wire-wire junction resistance in the AgNW film is a critical parameter to the electrical performance, and several techniques of nanowelding or soldering have been reported to reduce the wire-wire junction resistance. However, these methods require either specific facilities, or additional materials as the "solder", and often have adverse effects to the AgNW film or substrate. In this study, we show that at the nanoscale, capillary force is a powerful driving force that can effectively cause self-limited cold welding of the wire-wire junction for AgNWs. The capillary-force-induced welding can be simply achieved by applying moisture on the AgNW film, without any technical support like the addition of materials or the use of specific facilities. The moisture-treated AgNW films exhibit a significant decrease in sheet resistance, but negligible changes in transparency. We have also demonstrated that this method is effective to heal damaged AgNW films of wearable electronics and can be conveniently performed not only indoors but also outdoors where technical support is often unavailable. The capillary-force-based method may also be useful in the welding of other metal NWs, the fabrication of nanostructures, and smart assemblies for versatile flexible optoelectronic applications.

Nanoscale Back Contact Perovskite Solar Cell Design for Improved Tandem Efficiency.

Tandem photovoltaics, combining absorber layers with two distinct band gap energies into a single device, provide a practical solution to reduce thermalization losses in solar energy conversion. Traditionally, tandem devices have been assembled using two-terminal (2-T) or four-terminal (4-T) configurations; the 2-T limits the tandem performance due to the series connection requiring current matching, while the standard 4-T configuration requires at least three transparent electrical contacts, which reduce the total collected power due to unavoidable parasitic absorption. Here, we introduce a novel architecture based on a nanoscale back-contact for a thin-film top cell in a three terminal (3-T) configuration. Using coupled optical-electrical modeling, we optimize this architecture for a planar perovskite-silicon tandem, highlighting the roles of nanoscale contacts to reduce the required perovskite electronic quality. For example, with an 18% planar silicon base cell, the 3-T back contact design can reach a 32.9% tandem efficiency with a 10 µm diffusion length perovskite material. Using the same perovskite quality, the 4-T and 2-T configurations only reach 30.2% and 24.8%, respectively. We also confirm that the same 3-T efficiency advantage applies when using 25% efficient textured silicon base cells, where the tandems reach 35.2% and 32.8% efficiency for the 3-T, and 4-T configurations, respectively. Furthermore, because our design is based on the individual subcells being back-contacted, further improvements can be readily made by optimizing the front surface, which is left free for additional antireflective coating, light trapping, surface passivation, and photoluminescence outcoupling enhancements.

Development of a Novel Transparent Flexible Capacitive Micromachined Ultrasonic Transducer.

This paper presents the world's first transparent flexible capacitive micromachined ultrasonic transducer (CMUT) that was fabricated through a roll-lamination technique. This polymer-based CMUT has advantages of transparency, flexibility, and non-contacting detection which provide unique functions in display panel applications. Comprising an indium tin oxide-polyethylene terephthalate (ITO-PET) substrate, SU-8 sidewall and vibrating membranes, and silver nanowire transparent electrode, the transducer has visible-light transmittance exceeding 80% and can operate on curved surfaces with a 40 mm radius of curvature. Unlike the traditional silicon-based high temperature process, the CMUT can be fabricated on a flexible substrate at a temperature below 100 °C to reduce residual stress introduced at high temperature. The CMUT on the curved surfaces can detect a flat target and finger at distances up to 50 mm and 40 mm, respectively. The transparent flexible CMUT provides a better human-machine interface than existing touch panels because it can be integrated with a display panel for non-contacting control in a health conscious environment and the flexible feature is critical for curved display and wearable electronics.

Large-Scale Spinning of Silver Nanofibers as Flexible and Reliable Conductors.

Conducting metal nanowires can be assembled into thin films for flexible electronics and optoelectronics applications including transparent electrodes, nanocircuits, and electronic skin, however, the junction resistances and low aspect ratios still limit its performance. Herein we report high-quality silver nanofibers (AgNFs) synthesized by a gas-assistant solution spinning method. Compared with traditional Ag nanowires that usually have lengths below 100 µm, AgNFs are infinitely long and can be easily assembled into large-scale 2D and 3D flexible conductors with fused junctions between nanofibers. The AgNF networks showed high transparency, low sheet resistance (e. g, 6 Ω sq(-1) at ∼97% transparency), and high flexibility as transparent electrodes, whereas the 3D AgNF sponge could be used as a deformable and robust 3D conductor.

A transparent, solvent-free laminated top electrode for perovskite solar cells.

A simple lamination process of the top electrode for perovskite solar cells is demonstrated. The laminate electrode consists of a transparent and conductive plastic/metal mesh substrate, coated with an adhesive mixture of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate), PEDOT:PSS, and sorbitol. The laminate electrode showed a high degree of transparency of 85%. Best cell performance was achieved for laminate electrodes prepared with a sorbitol concentration of ~30 wt% per milliliter PEDOT:PSS dispersion, and using a pre-annealing temperature of 120°C for 10 min before lamination. Thereby, perovskite solar cells with stabilized power conversion efficiencies of (7.6 ± 1.0)% were obtained which corresponds to 80% of the reference devices with reflective opaque gold electrodes.