Low weight, small footprint, and high performances are essential requisites for the implementation of energy storage devices within consumer electronics. One way to achieve these goals is to increase the thickness of the active material layer. In this work, carbonized and graphitized rayon felt, a cellulose-derived material, is used as a three-dimensional current collector scaffold to enable the incorporation of large amount of active energy storage materials and ionic liquid-based gel electrolyte in the supercapacitor devices. PEDOT:PSS, alone or in combination with active carbon, has been used as the active material. Three-dimensional supercapacitors with high per unit area capacitance (more than 1.1 F/cm(2)) have been achieved owing to the loading of large amount of active material in the felt matrix. Areal energy density of more than 101 mu Wh/cm(2) and areal power density of more than 5.9 mW/cm(2) have been achieved for 0.8 V operating voltage at a current density of 1 mA/cm(2). A nanographite material was found to be beneficial in reducing the internal serial resistance of the supercapacitor to lower than 1.7 omega. Furthermore, it was shown that even after 2000 times cycling test, the devices could still retain its performance with at least 88% coulombic efficiency for all the devices. All the materials are readily available commercially, environmentally sustainable and the process can potentially be upscaled with industrial process.

A flexible, electrochromic, active matrix addressed display (AMAD) is demonstrated. The monolithically integrated AMAD, which contains a 3 × 3 array of organic electrochromic smart pixels (OESPs), is manufactured on a plastic substrate solely using screen printing. Each OESP is based on the combination of one organic electrochromic display (OECD) and one organic electrochemical transistor (OECT), where both devices are screen printed into multilayered vertical architectures. The conduction state of the OECT enables control of the color state of its corresponding OECD, thereby circumventing cross‐talk effects in the resulting AMAD device. The manufacturing approach also involves electrical wires, which connect each OECD with its corresponding OECT and also serve as the addressing lines of the resulting AMAD device, that are formed by screen printing of an ink based on either silver or nanocopper.

Body area networks (BANs), cloud computing, and machine learning are platforms that can potentially enable advanced healthcare outside the hospital. By applying distributed sensors and drug delivery devices on/in our body and connecting to such communication and decision-making technology, a system for remote diagnostics and therapy is achieved with additional autoregulation capabilities. Challenges with such autarchic on-body healthcare schemes relate to integrity and safety, and interfacing and transduction of electronic signals into biochemical signals, and vice versa. Here, we report a BAN, comprising flexible on-body organic bioelectronic sensors and actuators utilizing two parallel pathways for communication and decision-making. Data, recorded from strain sensors detecting body motion, are both securely transferred to the cloud for machine learning and improved decision-making, and sent through the body using a secure body-coupled communication protocol to auto-actuate delivery of neurotransmitters, all within seconds. We conclude that both highly stable and accurate sensing-from multiple sensors-are needed to enable robust decision making and limit the frequency of retraining. The holistic platform resembles the self-regulatory properties of the nervous system, i.e., the ability to sense, communicate, decide, and react accordingly, thus operating as a digital nervous system.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Here, we report all-screen printed display driver circuits, based on organic electrochemical transistors (OECTs), and their monolithic integration with organic electrochromic displays (OECDs). Both OECTs and OECDs operate at low voltages and have similar device architectures, and, notably, they rely on the very same electroactive material as well as on the same electrochemical switching mechanism. This then allows us to manufacture OECT-OECD circuits in a concurrent manufacturing process entirely based on screen printing methods. By taking advantage of the high current throughput capability of OECTs, we further demonstrate their ability to control the light emission in traditional light-emitting diodes (LEDs), where the actual LED addressing is achieved by an OECT-based decoder circuit. The possibility to monolithically integrate all-screen printed OECTs and OECDs on flexible plastic foils paves the way for distributed smart sensor labels and similar Internet of Things applications.

The communication outposts of the emerging Internet of Things are embodied by ordinary items, which desirably include all-printed flexible sensors, actuators, displays and akin organic electronic interface devices in combination with silicon-based digital signal processing and communication technologies. However, hybrid integration of smart electronic labels is partly hampered due to a lack of technology that (de)multiplex signals between silicon chips and printed electronic devices. Here, we report all-printed 4-to-7 decoders and seven-bit shift registers, including over 100 organic electrochemical transistors each, thus minimizing the number of terminals required to drive monolithically integrated all-printed electrochromic displays. These relatively advanced circuits are enabled by a reduction of the transistor footprint, an effort which includes several further developments of materials and screen printing processes. Our findings demonstrate that digital circuits based on organic electrochemical transistors (OECTs) provide a unique bridge between all-printed organic electronics (OEs) and low-cost silicon chip technology for Internet of Things applications.

Epindolidione, a hydrogen-bonded derivative of the organic semiconductor tetracene, is an organic pigment which has previously been used to produce stable OFETs with relatively high hole mobilities. Despite its use as an inkjet pigment and organic semiconductor, the crystal structure of epindolidione has proved elusive and is currently unknown. In this work, we report a crystal structure solution of epindolidione determined from vapor deposited thin films using a combined experimental and theoretical approach. The structure is found to be similar to one of the previously reported epindolidione derivatives and is most likely a surface-mediated polymorph, with a slightly different crystal packing compared to the bulk powder. The effect of substrate temperature on film morphology and structure is also investigated, where it is found that the crystallite orientation can be tuned by deposition at different substrate temperatures. The results also illustrate the possibilities for crystal structures to be solved from thin films.

We report on in situ performance evaluations as a function of layer thickness and substrate temperature for bottom-gate, bottom-gold contact epindolidione organic thin-film transistors on various gate dielectrics. Experiments were carried out under ultra-high vacuum conditions, enabling quasi simultaneous electrical and surface analysis. Auger electron spectroscopy and thermal desorption spectroscopy (TDS) were applied to characterize the quality of the substrate surface and the thermal stability of the organic films. Ex situ atomic force microscopy (AFM) was used to gain additional information on the layer formation and surface morphology of the hydrogen-bonded organic pigment. The examined gate dielectrics included SiO2, in its untreated and sputtered forms, as well as the spin coated organic capping layers poly(vinyl-cinnamate) (PVCi) and poly((+/-)endo,exo-bicyclo[2.2.1]hept-5-ene-2,3-dicarboxylic acid, diphenylester) (PNDPE, from the class of polynorbornenes). TDS and AFM revealed Volmer-Weber island growth dominated film formation with no evidence of a subjacent wetting layer. This growth mode is responsible for the comparably high coverage required for transistor behavior at 90-95% of a monolayer composed of standing molecules. Surface sputtering and an increased sample temperature during epindolidione deposition augmented the surface diffusion of adsorbing molecules and therefore led to a lower number of better-ordered islands. Consequently, while the onset of charge transport was delayed, higher saturation mobility was obtained. The highest, bottom-contact configuration, mobilities of approximately 2.5 x 10(-3)cm(2)/Vs were found for high coverages (50 nm) on sputtered samples. The coverage dependence of the mobility showed very different characteristics for the different gate dielectrics, while the change of the threshold voltage with coverage was approximately the same for all systems. An apparent decrease of the mobility with increasing coverage on the less polar PNDPE was attributed to a change in molecular orientation from upright standing in the thin-film phase to tilted in the bulk phase. From temperature-dependent mobility measurements we calculated activation barriers for the charge transport between 110 meV and 160 meV, depending on the dielectric configuration. (C) 2016 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license.

The evaporation of quinacridone from a stainless steel Knudsen cell leads to the partial decomposition of this molecule in the cell, due to its comparably high sublimation temperature. At least one additional type of molecules, namely indigo, could be detected in the effusion flux. Thermal desorption spectroscopy and atomic force microscopy have been used to study the co-deposition of these molecules on sputter-cleaned and carbon-covered silicon dioxide surfaces. Desorption of indigo appears at temperatures of about 400 K, while quinacridone desorbs at around 510 K. For quinacridone, a desorption energy of 2.1 eV and a frequency factor for desorption of 1 × 10(19) s(-1) were calculated, which in this magnitude is typical for large organic molecules. A fraction of the adsorbed quinacridone molecules (∼5%) decomposes during heating, nearly independent of the adsorbed amount, resulting in a surface composed of small carbon islands. The sticking coefficients of indigo and quinacridone were found to be close to unity on a carbon covered SiO2 surface but significantly smaller on a sputter-cleaned substrate. The reason for the latter can be attributed to insufficient energy dissipation for unfavorably oriented impinging molecules. However, due to adsorption via a hot-precursor state, the sticking probability is increased on the surface covered with carbon islands, which act as accommodation centers.

We report on the electrical in-situ characterisation of organic thin film transistors under high vacuum conditions. Model devices in a bottom-gate/bottom-contact (coplanar) configuration are electrically characterised in-situ, monolayer by monolayer (ML), while the organic semiconductor (OSC) is evaporated by organic molecular beam epitaxy (OMBE). Thermal SiO2 with an optional polymer interface stabilisation layer serves as the gate dielectric and pentacene is chosen as the organic semiconductor. The evolution of transistor parameters is studied on a bi-layer dielectric of a 150 nm of SiO2 and 20 nm of poly((±)endo,exo-bicyclo[2.2.1]hept-5-ene-2,3-dicarboxylic acid, diphenylester) (PNDPE) and compared to the behaviour on a pure SiO2 dielectric. The thin layer of PNDPE, which is an intrinsically photo-patternable organic dielectric, shows an excellent stabilisation performance, significantly reducing the calculated interface trap density at the OSC/dielectric interface up to two orders of magnitude, and thus remarkably improving the transistor performance.

In this work we present in situ electrical and surface analytical, as well as ex situ atomic force microscopy (AFM) studies on temperature and surface condition induced pentacene layer growth modifications, leading to the selection of optimized deposition conditions and entailing performance improvements. We prepared p++-silicon/silicon dioxide bottom-gate, gold bottom-contact transistor samples and evaluated the pentacene layer growth for three different surface conditions (sputtered, sputtered+carbon and unsputtered+carbon) at sample temperatures during deposition of 200K, 300K and 350K. The AFM investigations focused on the gold contacts, the silicon dioxide channel region and the highly critical transition area. Evaluations of coverage dependent saturation mobilities, threshold voltages and corresponding AFM analysis were able to confirm that the first 3–4 full monolayers contribute to the majority of charge transport within the channel region. At high temperatures and on sputtered surfaces uniform layer formation in the contact–channel transition area is limited by dewetting, leading to the formation of trenches and the partial development of double layer islands within the channel region instead of full wetting layers. By combining the advantages of an initial high temperature deposition (well-ordered islands in the channel) and a subsequent low temperature deposition (continuous film formation for low contact resistance) we were able to prepare very thin (8ML) pentacene transistors of comparably high mobility.

The fabrication of organic thin film transistors with highly reproducible characteristics presents a very challenging task. We have prepared and analyzed model pentacene thin film transistors under ultra-high vacuum conditions, employing surface analytical tools and methods. Intentionally contaminating the gold contacts and SiO2 channel area with carbon through repeated adsorption, dissociation, and desorption of pentacene proved to be very advantageous in the creation of devices with stable and reproducible parameters. We mainly focused on the device properties, such as mobility and threshold voltage, as a function of film morphology and preparation temperature. At 300 K, pentacene displays Stranski-Krastanov growth, whereas at 200 K fine-grained, layer-like film growth takes place, which predominantly influences the threshold voltage. Temperature dependent mobility measurements demonstrate good agreement with the established multiple trapping and release model, which in turn indicates a predominant concentration of shallow traps in the crystal grains and at the oxide-semiconductor interface. Mobility and threshold voltage measurements as a function of coverage reveal that up to four full monolayers contribute to the overall charge transport. A significant influence on the effective mobility also stems from the access resistance at the gold contact-semiconductor interface, which is again strongly influenced by the temperature dependent, characteristic film growth mode.