Abstract
Large-area single-crystalline thin films of n-type organic semiconductors (OSCs) fabricated via solution-processed techniques are urgently demanded for high-end electronics. However, the lack of molecular designs that concomitantly offer excellent charge-carrier transport, solution-processability, and chemical/thermal robustness for n-type OSCs limits the understanding of fundamental charge-transport properties and impedes the realization of large-area electronics. The benzo[de]isoquinolino[1,8-gh]quinolinetetracarboxylic diimide (BQQDI) π-electron system with phenethyl substituents (PhC(2) -BQQDI) demonstrates high electron mobility and robustness but its strong aggregation results in unsatisfactory solubility and solution-processability. In this work, an asymmetric molecular design approach is reported that harnesses the favorable charge transport of PhC(2) -BQQDI, while introducing alkyl chains to improve the solubility and solution-processability. An effective synthetic strategy is developed to obtain the target asymmetric BQQDI (PhC(2) -BQQDI-C(n) ). Interestingly, linear alkyl chains of PhC(2) -BQQDI-C(n) (n = 5-7) exhibit an unusual molecular mimicry geometry with a gauche conformation and resilience to dynamic disorders. Asymmetric PhC(2) -BQQDI-C(5) demonstrates excellent electron mobility and centimeter-scale continuous single-crystalline thin films, which are two orders of magnitude larger than that of PhC(2) -BQQDI, allowing for the investigation of electron transport anisotropy and applicable electronics.