Rational Design of Fluorinated 2D Polymer Film Based on Donor–Accepter Architecture toward Multilevel Memory Device for Neuromorphic Computing

Abstract Fluorine‐containing 2D polymer (F‐2DP) film is a desired system to regulate the charge transport in organic electronics but rather rarely reports due to the limited fluorine‐containing building blocks and difficulties in synthesis. Herein, a novel polar molecule with antiparallel columnar stacking is synthesized and further embedded into an F‐2DP system to control over the crystallinity of F‐2DP film through self‐complementary π ‐electronic forces. The donor–accepter–accepter′–donor′ (D–A–A′–D′) structure regulates the charge transportation efficiently, inducing multilevel memory behavior through stepwise charge capture and transfer processes. Thus, the device exhibits ternary memory behavior with low threshold voltage ( V th1 of 1.1 V, V th2 of 2.0 V), clearly distinguishable resistance states (1:10 2 :10 4 ) and ternary yield (83%). Furthermore, the stepwise formation of the charge complex endows the device with a wider range to regulate the conductive state, which allows its application in brain‐inspired neuromorphic computing. Modified National Institute of Standards and Technology recognition can reach an accuracy of 86%, showing great potential in neuromorphic computing applications in the post‐Moore era.