Unlocking the Potential of Ferrocene‐Functionalized Donor–π–Acceptor Systems with Phthalimide/Naphthalimide Acceptors for Non‐volatile Memory Devices

A series of donor–π–acceptor (D–π–A) push‐pull compounds incorporating ferrocene as the electron donor and phthalimide/naphthalimide as electron acceptors are designed and synthesized for nonvolatile memory applications. These compounds exhibit excellent solubility in common organic solvents, ensuring suitability for solution‐processed device fabrication. The strong donor–acceptor interactions in the D–π–A architecture enable efficient charge injection and transfer, essential for write‐once‐read‐many memory behavior. Among the synthesized compounds, a naphthalimide derivative with a trimethoxyphenyl substituent shows superior performance, with a low threshold voltage of −1.1 V, a high ON/OFF ratio (≈10 4 ), and a retention time of 2000 s. Systematic studies using optical, electrochemical, and theoretical analyses reveal that functional group modifications on the acceptor significantly influenced the electronic properties, particularly tuning the HOMO–LUMO gap (2.8–3.1 eV). These variations affect charge transport and bistable switching characteristics. Electrochemical measurements confirm the ferrocene core's redox‐active nature and acceptor units’ key role in enabling bistability. Theoretical simulations further elucidate charge trapping and release mechanisms. Overall, this work highlights the potential of ferrocene‐based D–π–A systems for next‐generation organic memory devices and provides valuable insights into structure–property relationships governing device performance.