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Triple Acceptors in a Polymeric Architecture for Balanced Ambipolar Transistors and High‐Gain Inverters

The exploration of novel molecular architectures is crucial for the design of high‐performance ambipolar polymer semiconductors. Here, a “triple‐acceptors architecture” strategy to design the ambipolar polymer DPP‐2T‐DPP‐TBT is introduced. The utilization of this architecture enables DPP‐2T‐DPP‐TBT to achieve deep‐lying highest occupied molecular orbital (HOMO)/lowest unoccupied molecular orbital (LUMO) levels of −5.38/−4.19 eV, and strong intermolecular interactions, which are favorable for hole/electron injection and intermolecular hopping through π‐stacking. All these factors result in excellent ambipolar transport characteristics and promising applications in complementary‐like circuits for DPP‐2T‐DPP‐TBT under ambient conditions with high hole/electron mobilities and a gain value of up to 3.01/3.84 cm2 V−1 s−1 and 171, respectively, which are among the best performances in ambipolar polymer organic thin‐film transistors and associated complementary‐like circuits, especially in top‐gate device configuration with low‐cost glass as substrates. These results demonstrate that the “triple‐acceptors architecture” strategy is an effective way for designing high‐performance ambipolar polymer semiconductors.