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Comprehensive Summary: Deep ultraviolet (UV) photodetectors have important applications in the industrial and military fields. However, little research has been reported on organic phototransistors (OPTs) in the deep ultraviolet range. Here, a novel organic semiconductor containing a small torsion angle and low π‐conjugation 2,2':5',2"‐terthiophene groups, oF‐PTTTP, is designed and synthesized, which exhibits high carrier mobility and unique deep ultraviolet response. Accordingly, an OPT based on oF‐PTTTP single crystal shows high responsivity to deep‐UV light. The photodetectors achieve high photoresponsivity (R) of 857 A/W and detectivity (D*) of 3.2×1015 Jones under 280 nm light illumination (only 95 nW·cm–2). To the best of our knowledge, 280 nm is the deepest detection wavelength reported for organic phototransistors and this work presents a new molecule design concept for organic phototransistors with deep‐UV detection. [ABSTRACT FROM AUTHOR]

Organic semiconductors with combinative high carrier mobility and efficient solid‐state emission are full of challenges but urgently pursued for developing new emerging optoelectronics. Herein, by delicately regulating the crystal packing of an anthracene‐based molecular crystal via terminal tert‐butylation, we developed a superior high mobility emissive molecule, 2,6‐di(6‐tert‐butylnaphthyl)anthracene (TBU‐DNA). The unique "slipped herringbone" packing motif of TBU‐DNA enables its appropriate exciton‐exciton coupling and electron‐phonon coupling, thus resulting in remarkably high solid‐state emission (photoluminescence quantum yield, ΦF≈74.9 %) and efficacious charge transport (carrier mobility, μ=5.0 cm2 V−1 s−1). Furthermore, OLETs based on TBU‐DNA show an external quantum efficiency (EQE) of 1.8 %, which is among the highest EQE values for single component OLETs reported till now. This work presents a crystal engineering strategy via exquisite molecular design to realize high mobility emissive organic semiconductors. [ABSTRACT FROM AUTHOR]

Organic semiconductors with combinative high carrier mobility and efficient solid‐state emission are full of challenges but urgently pursued for developing new emerging optoelectronics. Herein, by delicately regulating the crystal packing of an anthracene‐based molecular crystal via terminal tert‐butylation, we developed a superior high mobility emissive molecule, 2,6‐di(6‐tert‐butylnaphthyl)anthracene (TBU‐DNA). The unique "slipped herringbone" packing motif of TBU‐DNA enables its appropriate exciton‐exciton coupling and electron‐phonon coupling, thus resulting in remarkably high solid‐state emission (photoluminescence quantum yield, ΦF≈74.9 %) and efficacious charge transport (carrier mobility, μ=5.0 cm2 V−1 s−1). Furthermore, OLETs based on TBU‐DNA show an external quantum efficiency (EQE) of 1.8 %, which is among the highest EQE values for single component OLETs reported till now. This work presents a crystal engineering strategy via exquisite molecular design to realize high mobility emissive organic semiconductors. [ABSTRACT FROM AUTHOR]