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DOI: 10.1002/adma. 201400056 could form D–A complexes with tetracyanoquinodimethane (TCNQ)[10] and fullerenes [11] through a solution procedure. All these co-crystals displayed efficient ambipolar transport properties. In the former case, DPTTA and TCNQ stack alternatively into columns to form ribbon-shaped microcrystals, which display air-stable and balanced ambipolar transport properties with electron and hole mobilities up to 0.03 and 0.0 cm 2 V− 1 s− 1. Such behavior is rationalized by quantum calculations on superexchange effects in the intermolecular electronic couplings and molecular reorganization energy. In the latter cases, DPTTA and fullerenes (C60, C70) formed 2D segregated alternating layer structures, where continuing π–π interactions existed both in donor and acceptor layers, which serve as transport paths for holes and electrons, separately. These experimental and theoretical works revealed that D–A complexes with either mixed-or segregated-stack structures could be ambipolar semiconductors, and have stimulated continuous efforts in developing ambipolar materials with this combinational approach besides chemical tailoring strategies. Recently, more D–A co-crystals with ambipolar behavior were realized. Wakahara et al. reported a ambipolar transistor based on C 60-cobalt porphyrin (1: 1) co-crystal which displayed a balance of electron and hole mobilities in the range of 10− 5–10− 6 cm 2 V− 1 s− 1.[12] Park et al. developed a isometric donor–acceptor co-crystal with donor and acceptor molecules both based on distyrylbenzene, which displayed strong red emission property as well as p-/n-type field-effect …