Two anthracene‐based star‐shaped conjugated small molecules, 5′,5″‐(9,10‐bis((4‐hexylphenyl)ethynyl)anthracene‐2,6‐diyl)bis(5‐hexyl‐2,2′‐bithiophene), HBantHBT, and 5′,5″‐(9,10‐bis(phenylethynyl)anthracene‐2,6‐diyl)bis(5‐hexyl‐2,2′‐bithiophene), BantHBT, are used as electron‐cascade donor materials by incorporating them into organic photovoltaic cells prepared using a poly((5,5‐E‐alpha‐((2‐thienyl)methylene)‐2‐thiopheneacetonitrile)‐alt‐2,6‐[(1,5‐didecyloxy)naphthalene])) (PBTADN):[6,6]‐phenyl‐C71‐butyric acid methyl ester (PC71BM) blend. The small molecules penetrate the PBTADN:PC71BM blend layer to yield complementary absorption spectra through appropriate energy level alignment and optimal domain sizes for charge carrier transfer. A high short‐circuit current (JSC) and fill factor (FF) are obtained using solar cells prepared with the ternary blend. The highest photovoltaic performance of the PBTADN:BantHBT:PC71BM blend solar cells is characterized by a JSC of 11.0 mA cm−2, an open circuit voltage (VOC) of 0.91 V, a FF of 56.4%, and a power conversion efficiency (PCE) of 5.6% under AM1.5G illumination (with a high intensity of 100 mW−2). The effects of the small molecules on the ternary blend are investigated by comparison with the traditional poly(3‐hexylthiophene) (P3HT):[6,6]‐phenyl‐C61‐butyric acid methyl ester (PC61BM) system.
Interdependence of chemical structure, thin-film morphology, and transport properties is a key, yet often elusive aspect characterizing the design and development of high-mobility, solution-processed polymers for large-area and flexible electronics applications. There is a specific need to achieve >1 cm 2 V −1 s −1 field-effect mobilities (μ) at low processing temperatures in combination with environmental stability, especially in the case of electron-transporting polymers, which are still lagging behind hole transporting materials. Here, the synthesis of a naphthalene-diimide based donor-acceptor copolymer characterized by a selenophene vinylene selenophene donor moiety is reported. Optimized field-effect transistors show maximum μ of 2.4 cm 2 V −1 s −1 and promising ambient stability. A very marked film structural evolution is revealed with increasing annealing temperature, with evidence of a remarkable 3D crystallinity above 180 °C. Conversely, transport properties are found to be substantially optimized at 150 °C, with limited gain at higher temperature. This discrepancy is rationalized by the presence of a surface-segregated prevalently edge-on packed polymer phase, dominating the device accumulated channel. This study therefore serves the purpose of presenting a promising, high-electron-mobility copolymer that is processable at relatively low temperatures, and of clearly highlighting the necessity of specifically investigating channel morphology in assessing the structure-property nexus in semiconducting polymer thin films.
A universal method that enables utilization of conventional photolithography for processing a variety of polymer semiconductors is developed. The method relies on imparting chemical and physical orthogonality to a polymer film via formation of a semi‐interpenetrating diphasic polymer network with a bridged polysilsesquioxane structure, which is termed an orthogonal polymer semiconductor gel. The synthesized gel films remain tolerant to various chemical and physical etching processes involved in photolithography, thereby facilitating fabrication of high‐resolution patterns of polymer semiconductors. This method is utilized for fabricating tandem electronics, including pn‐complementary inverter logic devices and pixelated polymer light‐emitting diodes, which require deposition of multiple polymer semiconductors through solution processes. This novel and universal method is expected to significantly influence the development of advanced polymer electronics requiring sub‐micrometer tandem structures.
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