Fullerene/Sulfur-Bridged Annulene Cocrystals: Two-Dimensional Segregated Heterojunctions with Ambipolar Transport Properties and Photoresponsivity

Fullerene/sulfur-bridged annulene cocrystals with a two-dimensional segregated alternating layer structure were prepared by a simple solution process. Single-crystal analysis revealed the existence of continuing π–π interactions in both the donor and acceptor layers, which serve as transport paths for holes and electrons separately. The ambipolar transport behaviors were demonstrated with single-crystal field-effect transistors and rationalized by quantum calculations. Meanwhile, preliminary photoresponsivity was observed with the transistor configuration.