The optical, structural, and electrical properties of thin layers made from poly(3‐hexylthiophene) (P3HT) samples of different molecular weights are presented. As reported in a previous paper by Kline et al., Adv. Mater. 2003, 15, 1519, the mobilities of these layers are a strong function of the molecular weight, with the largest mobility found for the largest molecular weight. Atomic force microscopy studies reveal a complex polycrystalline morphology which changes considerably upon annealing. X‐ray studies show the occurrence of a layered phase for all P3HT fractions, especially after annealing at 150 °C. However, there is no clear correlation between the differences in the transport properties and the data from structural investigations. In order to reveal the processes limiting the mobility in these layers, the transistor properties were investigated as a function of temperature. The mobility decreases continuously with increasing temperatures; with the same trend pronounced thermochromic effects of the P3HT films occur. Apparently, the polymer chains adopt a more twisted, disordered conformation at higher temperatures, leading to interchain transport barriers. We conclude that the backbone conformation of the majority of the bulk material rather than the crystallinity of the layer is the most crucial parameter controlling the charge transport in these P3HT layers. This interpretation is supported by the significant blue‐shift of the solid‐state absorption spectra with decreasing molecular weight, which is indicative of a larger distortion of the P3HT backbone in the low‐molecular weight P3HT layers.
The cost-effective production of flexible electronic components will profit considerably from the development of solution-processable, organic semiconductor materials. Particular attention is focused on soluble semiconductors for organic field-effect transistors (OFETs). The hitherto differentiation between "small molecules" and polymeric materials no longer plays a role, rather more the ability to process materials from solution to homogeneous semiconducting films with optimal electronic properties (high charge-carrier mobility, low threshold voltage, high on/off ratio) is pivotal. Key classes of materials for this purpose are soluble oligoacenes, soluble oligo- and polythiophenes and their respective copolymers, and oligo- and polytriarylamines. In this context, micro- or nanocrystalline materials have the general advantage of somewhat higher charge-carrier mobilities, which, however, could be offset in the case of amorphous, glassy materials by simpler and more reproducible processing.
There is ample evidence that organic field-effect transistors have reached a stage where they can be industrialized, analogous to standard metal oxide semiconductor (MOS) transistors. Monocrystalline silicon technology is largely based on complementary MOS (CMOS) structures that use both n-type and p-type transistor channels. This complementary technology has enabled the construction of digital circuits, which operate with a high robustness, low power dissipation and a good noise margin. For the design of efficient organic integrated circuits, there is an urgent need for complementary technology, where both n-type and p-type transistor operation is realized in a single layer, while maintaining the attractiveness of easy solution processing. We demonstrate, by using solution-processed field-effect transistors, that hole transport and electron transport are both generic properties of organic semiconductors. This ambipolar transport is observed in polymers based on interpenetrating networks as well as in narrow bandgap organic semiconductors. We combine the organic ambipolar transistors into functional CMOS-like inverters.
A Bose-Einstein condensate (BEC) is a state of matter in which extensive collective coherence leads to intriguing macroscopic quantum phenomena. In crystalline semiconductor microcavities, bosonic quasiparticles, known as exciton-polaritons, can be created through strong coupling between bound electron-hole pairs and the photon field. Recently, a non-equilibrium BEC (ref. ) and superfluidity have been demonstrated in such structures. With organic crystals grown inside dielectric microcavities, signatures of polariton lasing have been observed. However, owing to the deleterious effects of disorder and material imperfection on the condensed phase, only crystalline materials of the highest quality have been used until now. Here we demonstrate non-equilibrium BEC of exciton-polaritons in a polymer-filled microcavity at room temperature. We observe thermalization of polaritons and, above a critical excitation density, clear evidence of condensation at zero in-plane momentum, namely nonlinear behaviour, blueshifted emission and long-range coherence. The key signatures distinguishing the behaviour from conventional photon lasing are presented. As no crystal growth is involved, our approach radically reduces the complexity of experiments to investigate BEC physics and paves the way for a new generation of opto-electronic devices, taking advantage of the processability and flexibility of polymers.
Keto defect sites play a key role as the source of low‐energy emission bands in polyfluorene type materials. The formation of fluorenone defect sites can be regarded as a dominant degradation mechanism in light‐emitting devices based on polyfluorenes. The superiority of difunctionalization (see Figure) at the methylene group in –CR2– bridged polyphenylene and polyarylene derivatives is illustrated.
Atomically dispersed transition metal active sites have emerged as one of the most important fields of study because they display promising performance in catalysis and have the potential to serve as ideal models for fundamental understanding. However, both the preparation and determination of such active sites remain a challenge. The structural engineering of carbon-and nitrogencoordinated metal sites (M−N−C, M = Fe, Co, Ni, Mn, Cu, etc.) via employing new heteroatoms, e.g., P and S, remains challenging. In this study, carbon nanosheets embedded with nitrogen and phosphorus dual-coordinated iron active sites (denoted as Fe-N/P-C) were developed and determined using cutting edge techniques. Both experimental and theoretical results suggested that the N and P dual-coordinated iron sites were favorable for oxygen intermediate adsorption/desorption, resulting in accelerated reaction kinetics and promising catalytic oxygen reduction activity. This work not only provides efficient way to prepare well-defined single-atom active sites to boost catalytic performance but also paves the way to identify the dual-coordinated single metal atom sites.
Recently, two different groups have reported independently that the mobility of field-effect transistors made from regioregular poly(3-hexylthiophene) (P3HT) increases strongly with molecular weight. Two different models were presented: one proposing carrier trapping at grain boundaries and the second putting emphasis on the conformation and packing of the polymer chains in the thin layers for different molecular weights. Here, we present the results of detailed investigations of powders and thin films of deuterated P3HT fractions with different molecular weight. For powder samples, gel permeation chromatography (GPC), differential scanning calorimetry (DSC), and X-ray diffraction (XRD) were used to investigate the structure and crystallization behavior of the polymers. The GPC investigations show that all weight fractions possess a rather broad molecular weight distribution. DSC measurements reveal a strong decrease of the crystallization temperature and, most important, a significant decrease of the degree of crystallinity with decreasing molecular weight. To study the structure of thin layers in lateral and vertical directions, both transmission electron microscopy (TEM) and X-ray grazing incidence diffraction (GID) were utilized. These methods show that thin layers of the low molecular weight fraction consist of well-defined crystalline domains embedded in a disordered matrix. We propose that the transport properties of layers prepared from fractions of poly(3-hexylthiophene) with different molecular weight are largely determined by the crystallinity of the samples and not by the perfection of the packing of the chains in the individual crystallites.
The power conversion efficiencies of bulk heterojunction (BHJ) solar cells can be increased from 5 to 6.5% by incorporating an ultrathin conjugated polyelectrolyte (CPE) layer between the active layer and the metal cathode. Poly[N-9''-heptadecanyl-2,7-carbazole-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)] (PCDTBT) and [6,6]-phenyl C(71) butyric acid methyl ester (PC(71)BM) were chosen for the photoactive layer. CPEs with cationic polythiophenes, in both homopolymer and block copolymer configurations, were used to improve the electronic characteristics. The significant improvement in device performance and the simplicity of fabrication by solution processing suggest a promising and practical pathway for improving polymer solar cells with high efficiencies.
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