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There is a growing demand to attain organic materials with high electron mobility, μe, as current reliable reported values are significantly lower than those exhibited by their hole mobility counterparts. Here, it is shown that a well‐known nonfullerene‐acceptor commonly used in organic solar cells, that is, BTP‐4F (aka Y6), enables solution‐processed organic thin‐film transistors (OTFT) with a μe as high as 2.4 cm2 V−1 s−1. This value is comparable to those of state‐of‐the‐art n‐type OTFTs, opening up a plethora of new possibilities for this class of materials in the field of organic electronics. Such efficient charge transport is linked to a readily achievable highly ordered crystalline phase, whose peculiar structural properties are thoroughly discussed. This work proves that structurally ordered nonfullerene acceptors can exhibit intrinsically high mobility and introduces a new approach in the quest of high μe organic materials, as well as new guidelines for future materials design. n‐channel organic thin‐film transistors exhibiting electron mobility values as high as 2.4 cm2 V−1 s−1 are produced with the benchmark nonfullerene acceptor used in organic solar cell, that is, BTP‐4F (aka Y6). These properties stem from crystallization of Y6 in a crystalline structure featuring molecularly flat, highly ordered, and textured domains.

Copper(II) phthalocyanine (CuPc), also known as Pigment Blue 15, is a widely utilized pigment renowned for its exceptional semiconducting properties when refined to electronic‐grade purity. Recent studies have confirmed its safety if ingested at doses required for essential active components in edible electronics for advanced gastrointestinal tract monitoring. Since in‐body operations impose stringent safety constraints on operational biases, the development of transistors with high transconductance at low voltages is required to ensure adequate amplification gain. This study presents a simple and cost‐effective method for producing solution‐processed CuPc films characterized by a unique porous microstructure that facilitates efficient volumetric ion uptake and mixed ionic‐electronic conductivity in electrolyte‐gated devices. These porous films exhibit capacitance 30 times greater than compact CuPc films produced through conventional physical vapor deposition methods. The resulting edible transistors demonstrate On/Off ratios exceeding 103 and channel width‐normalized transconductance of up to 50 µS mm−1 at 0.8 V, establishing their potential as critical active components in future edible devices. Moreover, the proposed method results in a limited impact of impurities on CuPc charge transport efficiency, thus affecting the purification costs and, crucially, enabling the sourcing of CuPc pigments through recycling and upcycling. A novel solution‐based method is presented to produce Copper Phthalocyanine fibrous films displaying effective ion permeability and enhanced transconductance in electrolyte‐gated transistors architectures. Using these films, the first instance of a fully edible electrolyte‐gated transistor with volumetric capacitance, targeting in‐body applications, is demonstrated. Additionally, the effective sourcing of CuPc is showcased from the upcycling of Pigment Blue 15.

The addition of a third component to a donor:acceptor blend is a powerful tool to enhance the power conversion efficiency of organic solar cells. Featuring a similar operating mechanism, organic photodetectors are also expected to benefit from this approach. Here, we fabricated ternary organic photodetectors, based on a polymer donor and two nonfullerene acceptors, resulting in a low dark current of 0.42 nA cm −2 at −2 V and a broadband specific detectivity of 10 12 Jones. We found that exciton recombination in the binary blend is reduced in ternary devices due to the formation of a pseudo-binary microstructure with mixed donor–acceptor phases. With this approach a wide range of intermediate open-circuit voltages is accessible, without sacrificing light-to-current conversion. This results in ternary organic photodetector (TOPD) with improved Responsivity values in the near-infrared. Moreover, morphology analyses reveal that TOPD devices showed improved microstructure ordering and consequentially higher charge carrier mobilities compared to the reference devices.

There is a growing demand to attain organic materials with high electron mobility, μ e , as current reliable reported values are significantly lower than those exhibited by their hole mobility counterparts. Here, it is shown that a well‐known nonfullerene‐acceptor commonly used in organic solar cells, that is, BTP‐4F (aka Y6), enables solution‐processed organic thin‐film transistors (OTFT) with a μ e as high as 2.4 cm 2  V −1  s −1 . This value is comparable to those of state‐of‐the‐art n‐type OTFTs, opening up a plethora of new possibilities for this class of materials in the field of organic electronics. Such efficient charge transport is linked to a readily achievable highly ordered crystalline phase, whose peculiar structural properties are thoroughly discussed. This work proves that structurally ordered nonfullerene acceptors can exhibit intrinsically high mobility and introduces a new approach in the quest of high μ e organic materials, as well as new guidelines for future materials design.

Solution-processed, large-area, and flexible electronics largely relies on the excellent electronic properties of sp\\(^2\\)-hybridized carbon molecules, either in the form of \\(\\pi\\)-conjugated small molecules and polymers or graphene and carbon nanotubes. Carbon with sp-hybridization, the foundation of the elusive allotrope carbyne, offers vast opportunities for functionalized molecules in the form of linear carbon atomic wires (CAWs), with intriguing and even superior predicted electronic properties. While CAWs represent a vibrant field of research, to date, they have only been applied sparingly to molecular devices. The recent observation of the field-effect in microcrystalline cumulenes suggests their potential applications in solution-processed thin-film transistors but concerns surrounding the stability and electronic performance have precluded developments in this direction. In the present study, ideal field-effect characteristics are demonstrated for solution-processed thin films of tetraphenyl[3]cumulene, the shortest semiconducting CAW. Films are deposited through a scalable, large-area, meniscus-coating technique, providing transistors with hole mobilities in excess of 0.1 cm\\(^2\\) V\\(^{-1}\\) s\\(^{-1}\\), as well as promising operational stability under dark conditions. These results offer a solid foundation for the exploitation of a vast class of molecular semiconductors for organic electronics based on sp-hybridized carbon systems and create a previously unexplored paradigm.

Indacenodithiophene (IDT) based materials are emerging high performance conjugated polymers for use in efficient organic photovoltaics and transistors. However, their preparation generally suffers from long reaction sequences and is often accomplished using disadvantageous Stille couplings. Herein, we present detailed synthesis pathways to IDT homopolymers using C-H activation for all C-C coupling steps. Polyketones are first prepared by direct arylation polycondensation (DAP) in quantitative yield and further cyclized polymer analogously. This protocol is suitable for obtaining structurally well-defined IDT homopolymers, provided that the conditions for cyclization are chosen appropriately and that side reactions are suppressed. Moreover, this polymer analogous pathway gives rise to asymmetric side chain patterns, which allows to fine tune physical properties. Alternatively, IDT homopolymers can be obtained via oxidative direct arylation polycondensation of IDT monomers (oxDAP), leading to IDT homopolymers with similar properties but at reduced yield. Detailed characterization by NMR, IR, UV-vis and PL spectroscopy, and thermal properties, is used to guide synthesis and to explain varying field-effect transistor hole mobilities in the range of 10-6- 10-3 cm2/Vs.

The high photoluminescence efficiency, color purity, extended gamut, and solution processability make low-dimensional hybrid perovskites attractive for light-emitting diode (PeLED) applications. However, controlling the microstructure of these materials to improve the device performance remains challenging. Here, the development of highly efficient green PeLEDs based on blends of the quasi-2D (q2D) perovskite, PEA2Cs4Pb5Br16, and the wide bandgap organic semiconductor 2,7 dioctyl[1] benzothieno[3,2-b]benzothiophene (C8-BTBT) is reported. The presence of C8-BTBT enables the formation of single-crystal-like q2D PEA2Cs4Pb5Br16 domains that are uniform and highly luminescent. Combining the PEA2Cs4Pb5Br16:C8-BTBT with self-assembled monolayers (SAMs) as hole-injecting layers (HILs), yields green PeLEDs with greatly enhanced performance characteristics, including external quantum efficiency up to 18.6%, current efficiency up to 46.3 cd/A, the luminance of 45 276 cd m^-2, and improved operational stability compared to neat PeLEDs. The enhanced performance originates from multiple synergistic effects, including enhanced hole-injection enabled by the SAM HILs, the single crystal-like quality of the perovskite phase, and the reduced concentration of electronic defects. This work highlights perovskite:organic blends as promising systems for use in LEDs, while the use of SAM HILs creates new opportunities toward simpler and more stable PeLEDs.