13 Search Results

The use of grazing-incidence scattering methods for the characterization of 2D patterned organic thin films is limited due to the elongated 1D footprint of the X-ray beam on the sample. However, this characteristic feature can be turned into an advantage, when combined with tomographic reconstruction. In this pilot study we show, how the use of a chosen texture reflection and a diffuse reflectivity signal can each provide 2D images of the deposits, simultaneously revealing the organic film's crystal orientation and the location of the metal electrodes in a field-effect transistor structure from a single sequence of diffraction images.

Abstract Controlling polymer chain alignment through processing is a means of tuning the charge transport of solution‐based conjugated polymers. In this work, a processing strategy is proposed in which an external electric field (E‐field) is applied to the coating blade (E‐blade) to align polymer chain during solution‐shearing, a meniscus‐guided coating technique. A theoretical model based on dielectrophoresis quantitatively describes and predicts the alignment process and is used to guide the selection of the optimal conditions of the applied E‐field. Using these conditions, more than twofold increase in chain alignment is observed for E‐bladed thin films of a diketopyrrolopyrrole (DPP) semiconductingmore » polymer without affecting other morphological aspects such as film thickness, film coverage, or fiber‐like aggregation. Organic field effect transistors based on the E‐bladed DPP polymer are fabricated at ambient conditions and over areas of a few cm ² . They display a threefold improvement in their mobilities and a strong enhancement in charge transport anisotropy compared to films prepared without E‐field. These results reveal a synergistic alignment effect from both the solution‐shearing process and the applied E‐field, and introduce a novel and general approach to control the morphology and the electrical properties of solution‐coated conjugated polymer thin films.« less

Stretchable semiconducting polymers have been developed as a key component to enable skin-like wearable electronics, but their electrical performance must be improved to enable more advanced functionalities. Here, we report a solution processing approach that can achieve multi-scale ordering and alignment of conjugated polymers in stretchable semiconductors to substantially improve their charge carrier mobility. Using solution shearing with a patterned microtrench coating blade, macroscale alignment of conjugated-polymer nanostructures was achieved along the charge transport direction. In conjunction, the nanoscale spatial confinement aligns chain conformation and promotes short-range π–π ordering, substantially reducing the energetic barrier for charge carrier transport. As amore » result, the mobilities of stretchable conjugated-polymer films have been enhanced up to threefold and maintained under a strain up to 100%. This method may also serve as the basis for large-area manufacturing of stretchable semiconducting films, as demonstrated by the roll-to-roll coating of metre-scale films.« less

Crucial to the development and refinement of organic electronics is a fundamental understanding of how deposition processes affect the active material’s resulting microstructure in the thin film. Meniscus-guided coating (MGC) methods are attractive because of their amenability to high-throughput, industrially relevant continuous processes like roll-to-roll deposition, but the mechanism of solid film formation has not been elucidated and is valuable for the precise control of thin-film morphology and thus ultimate device performance. Here, in this work, we investigate the microstructural evolution of thin films of a diketopyrrolopyrrole–terthiophene donor–acceptor polymer semiconductor using both in situ and ex situ X-ray diffraction methods.more » On the basis of a comparison of disorder between the film bulk and the top surface and a depth profiling of the out-of-plane orientation of crystallites, we find that faster coating speeds introduce more disorder into the resulting films because the stochastic nucleation of disordered crystallites at the meniscus air–liquid interface becomes more dominant than substrate-mediated nucleation. Our results suggest that there exist three separate deposition regimes—namely the shear-dominate, disorder-dominate, and Landau–Levich–Derjaguin regimes—revealed by observing both polymer alignment via dry film thickness and optical dichroism, a property sensitive to the flow and shear fields. At low coating speeds, the shear strain imparted upon the solution directly induces polymer alignment, causing an increase in dichroism as a function of coating speed. When solvent evaporation becomes too rapid as coating speeds increase, a decrease in the dichroic ratio is observed before the classical Landau–Levich–Derjaguin regime occurs at the highest coating speeds, resulting in isotropic films. The preservation of out-of-plane crystalline texture throughout the thickness of the films is seen only for lower coating speeds, and a study of different deposition temperatures similarly indicates that the lower overall solvent evaporation is conducive to this process. Increased paracrystalline disorder (i.e., peak broadening) is observed by grazing-incidence wide-angle X-ray diffraction at the top interface of the dry films and at higher coating speeds. Together, these results indicate that more rapid solvent evaporation at higher coating speeds causes increased disorder, which can cause the nucleation of misaligned crystallites, affect the dichroic ratio, and may frustrate the alignment of polymer molecules in the amorphous regions of the film. Finally, because the polymer studied and the deposition technique used are representative models, these results are likely general for aggregating, semicrystalline donor–acceptor polymers deposited with MGC.« less

The electronic devices that play a vital role in our daily life are primarily based on silicon and are thus rigid, opaque, and relatively heavy. However, new electronics relying on polymer semiconductors are opening up new application spaces like stretchable and self-healing sensors and devices, and these can facilitate the integration of such devices into our homes, our clothing, and even our bodies. So, while there has been tremendous interest in such technologies, the widespread adoption of these organic electronics requires low-cost manufacturing techniques. Fortunately, the realization of organic electronics can take inspiration from a technology developed since the beginningmore » of the Common Era: printing. Here, this review addresses the critical issues and considerations in the printing methods for organic electronics, outlines the fundamental fluid mechanics, polymer physics, and deposition parameters involved in the fabrication process, and provides future research directions for the next generation of printed polymer electronics.« less

For miniaturized capacitive energy storage, volumetric and areal capacitances are more important metrics than gravimetric ones because of the constraints imposed by device volume and chip area. Typically used in commercial supercapacitors, porous carbons, although they provide a stable and reliable performance, lack volumetric performance because of their inherently low density and moderate capacitances. Here we report a high-performing electrode based on conductive hexaaminobenzene (HAB)-derived two-dimensional metal-organic frameworks (MOFs). In addition to possessing a high packing density and hierarchical porous structure, these MOFs also exhibit excellent chemical stability in both acidic and basic aqueous solutions, which is in sharp contrastmore » to conventional MOFs. Submillimetre-thick pellets of HAB MOFs showed high volumetric capacitances up to 760 F cm(-3) and high areal capacitances over 20 F cm(-2). Furthermore, the HAB MOF electrodes exhibited highly reversible redox behaviours and good cycling stability with a capacitance retention of 90% after 12,000 cycles. These promising results demonstrate the potential of using redox-active conductive MOFs in energy-storage applications.« less

Significance Organic electronics, particularly polymers, can be synthesized and processed with low temperatures and, more importantly, have the potential to be environmentally benign candidates for electronic applications. However, there has been no report of totally decomposable polymer semiconductors. Their availability will enable low-cost and fully disintegrable transient electronics. We have developed an innovative concept based on imine chemistry that allows totally disintegrable and biocompatible semiconducting polymers. Using an ultrathin biodegradable substrate, we successfully fabricated polymer transistors and logic circuits that show high performance and are ultralightweight, but they can be fully disintegrable. Our work significantly advances organic materials to enablemore » environmentally friendly and biointegrated electronic applications.« less

The solid‐state packing and polymer orientation relative to the substrate are key properties to control in order to achieve high charge carrier mobilities in organic field effect transistors (OFET). Intuitively, shorter side chains are expected to yield higher charge carrier mobilities because of a denser solid state packing motif and a higher ratio of charge transport moieties. However our findings suggest that the polymer chain orientation plays a crucial role in high‐performing diketopyrrolopyrrole‐based polymers. By synthesizing a series of DPP‐based polymers with different branched alkyl side chain lengths, it is shown that the polymer orientation depends on the branched alkylmore » chain lengths and that the highest carrier mobilities are obtained only if the polymer adopts a mixed face‐on/edge‐on orientation, which allows the formation of 3D carrier channels in an otherwise edge‐on‐oriented polymer chain network. Time‐of‐flight measurements performed on the various polymer films support this hypothesis by showing higher out‐of‐plane carrier mobilities for the partially face‐on‐oriented polymers. Additionally, a favorable morphology is mimicked by blending a face‐on polymer into an exclusively edge‐on oriented polymer, resulting in higher charge carrier mobilities and opening up a new avenue for the fabrication of high performing OFET devices.« less

Organic field-effect transistors have attracted much attention because of their potential use in low-cost, large-area, flexible electronics. High-performance organic transistors require a low density of grain boundaries in their organic films and a decrease in the charge trap density at the semiconductor–dielectric interface for efficient charge transport. In this respect, the role of the dielectric material is crucial because it primarily determines the growth of the film and the interfacial trap density. Here, we demonstrate the use of chemical vapor-deposited hexagonal boron nitride (CVD h-BN) as a scalable growth template/dielectric for high-performance organic field-effect transistors. The field-effect transistors based onmore » C60 films grown on single-layer CVD h-BN exhibit an average mobility of 1.7 cm² V^–1 s^–1 and a maximal mobility of 2.9 cm² V^–1 s^–1 with on/off ratios of 10⁷. The structural and morphology analysis shows that the epitaxial, two-dimensional growth of C₆₀ on CVD h-BN is mainly responsible for the superior charge transport behavior. In conclusion, we believe that CVD h-BN can serve as a growth template for various organic semiconductors, allowing the development of large-area, high-performance flexible electronics.« less

Morphology control of solution coated solar cell materials presents a key challenge limiting their device performance and commercial viability. Here we present a new concept for controlling phase separation during solution printing using an all-polymer bulk heterojunction solar cell as a model system. The key aspect of our method lies in the design of fluid flow using a microstructured printing blade, on the basis of the hypothesis of flow-induced polymer crystallization. Our flow design resulted in a similar to 90% increase in the donor thin film crystallinity and reduced microphase separated donor and acceptor domain sizes. The improved morphology enhancedmore » all metrics of solar cell device performance across various printing conditions, specifically leading to higher short-circuit current, fill factor, open circuit voltage and significantly reduced device-to-device variation. However, we expect our design concept to have broad applications beyond all-polymer solar cells because of its simplicity and versatility.« less