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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]

Keywords: Charge Transport; Crystal Engineering; Light Emission; Molecular Crystals; Organic Semiconductor EN Charge Transport Crystal Engineering Light Emission Molecular Crystals Organic Semiconductor 1 1 1 11/03/22 20221107 NES 221107 B An anthracene-based molecular crystal b with a unique "slipped herringbone" packing motif was developed by crystal engineering through terminal I tert i -butylation. Appropriate exciton-exciton coupling/electron-phonon coupling originating from the unique crystal packing induces a remarkably strong solid-state emission and efficient charge transport, as reported by Wenping Hu et al. in their Research Article (e202206825). Appropriate exciton-exciton coupling/electron-phonon coupling originating from the unique crystal packing induces a remarkably strong solid-state emission and efficient charge transport, as reported by Wenping Hu et al. in their Research Article (e202206825). [Extracted from the article]