p-n heterojunctions composed of two-dimensional molecular crystals for high-performance ambipolar organic field-effect transistors

Bilayer p-n heterojunctions are promising structures to construct ambipolar organic field-effect transistors (aOFETs) for organic integrated circuits. However, due to the lack of effective strategies for high-quality p-n heterojunctions with clear interfaces, the performance of aOFETs is commonly and substantially lower than that of their unipolar counterparts, which hinders the development of aOFETs toward practical applications. Herein, a one-step solution crystallization strategy was proposed for the preparation of high-quality bilayer p-n heterojunctions. A mixed solution of a p- and an n-type organic semiconductor was dropped on a liquid substrate, and vertical phase separation occurred spontaneously during crystallization to produce bilayer p-n heterojunctions composed of molecularly thin two-dimensional molecular crystals. Due to the clear interface of the bilayer p-n heterojunctions, the maximum mobility (average mobility) reached 1.96 cm2 V−1 s−1 (1.12 cm2 V−1 s−1) for holes and 1.27 cm2 V−1 s−1 (0.61 cm2 V−1 s−1) for electrons in ambient air. So far as we know, these values were the highest among double-channel aOFETs measured in ambient air. This work provides a simple yet efficient strategy to construct high-quality bilayer p-n heterojunctions, which lays a foundation for their application in high-performance optoelectronic devices.