Developing high‐quality electret layer is important for the fabrication of high‐performance nonvolatile organic field effect transistor memory devices (OFET‐NVMs). In this work, three representative aromatic diimide frameworks are employed for comparative studies as n‐type doping materials for the electret layers in OFET‐NVMs, which are naphthalene diimide (NDI), perylene diimide (PDI), and pyrene diimide (PyDI). When blended with polystyrene (PS) to prepare the electret layers, all the memory devices containing aromatic diimide dopants exhibited significantly improved performances compared with the undoped counterparts, indicating that low‐lying LUMO energy levels of these dopants are beneficial for charge injection. All the devices with n‐type dopants exhibited long retention times (more than 104 s) and good switching reliability in more than 400 continuous write‐read‐erase‐read cycles. Among them, the PyDI‐based memory device exhibited superior performance compared with other aromatic diimides, which achieved a memory window of 34.0 V, a trapping charge density of 1.98 × 1012 cm−2 along with an on/off ratio higher than 104. This work indicates that PyDI framework could be a new platform for the future design of n‐type dopant for high‐performance nonvolatile organic field‐effect transistor memory devices.

Pyrazine-fused isoindigo (PzIIG) was designed and synthesized as a novel electron acceptor to construct two D-A conjugated polymers, PzIIG-BDT2TC8 and PzIIG-BTT2TC10. Both the polymers were successfully applied in polymer solar cells, and the PzIIG-BDT2TC8 based solar cell device exhibited a PCE of 5.26% with a high V over 1.0 V.