LAUSR

Donor–acceptor type polymers and supramolecules are promising electrets in photonic field‐effect transistor (FET)‐type memory because of their diversified polymer‐structure design and favorable mechanical tolerance. Using intermolecular association, supramolecule electrets can surpass donor–acceptor type polymers with versatile facile combining processes. Currently, there has been no application of charge‐transfer (CT) supramolecules in electrets of photonic FET memory devices. Herein, a novel series of CT‐based supramolecular electrets comprising poly(1‐pyrenemethyl methacrylate) (PPyMA) and 7,7,8,8‐tetracyanoquinodimethane (TCNQ) is used to elucidate the effect of CT on photonic FET memory. Accordingly, memory devices based on the supramolecular electret with an equimolar content of pyrene and TCNQ exhibit superior bistable memory switchability using electrical/photoprograming with UV (365 nm) and green light (525 nm). This shows a broad memory window of 34 V and favorable memory ratio of over 106 after 104 s. The memory performance can be attributed to the favorable molecular association and dispersion between pyrene and TCNQ in the solid state. The results provide evidence that CT‐based supramolecular electrets warrant applications in optoelectronic applications.