Molecularly Engineered Wing‐Shaped Azobenzene Memristors for Logic‐in‐Memory and Edge Visual Intelligence

ABSTRACT Organic molecular resistive memory offers a promising platform to overcome the von Neumann bottleneck. Here, we report four symmetric azobenzene‐based small molecules with diverse terminal substituents (nitroimidazole, imidazole, carbazole, and triphenylamine) for memristive applications. By tuning the terminal groups, the devices exhibit tunable nonvolatile behaviors—ranging from ternary/binary WORM to bipolar nonvolatile resistive memory—all featuring high ON/OFF ratios, low operating voltages, and excellent stability. Mechanistic studies reveal that charge‐transfer‐induced conformational changes govern the twisted intramolecular charge‐transfer states, dictating these distinct memory characteristics. Notably, the Cz‐methylene‐Azo memristor demonstrates continuous conductance tunability and essential synaptic functions (e.g., excitatory postsynaptic current (EPSC), paired‐pulse facilitation (PPF), long‐term potentiation/depression (LTP/D)). Furthermore, it serves as a versatile logic‐in‐memory unit, executing multiple logic gates (OR, AND, XOR, NAND, etc.), the half and full‐adder circuits. Its applicability for in‐memory computing is successfully validated via convolutional neural networks (CNN)‐based image edge detection, highlighting its great potential for next‐generation integrated organic neuromorphic architectures.