Electrosynthesis of Ru (II)-Polypyridyl Oligomeric Films on ITO Electrode for Two Terminal Non-Volatile Memory Devices and Neuromorphic Computing.

Molecular electronics exhibiting resistive-switching memory features hold great promise for the next generation of digital technology. In this work, electrosynthesis of ruthenium polypyridyl nanoscale oligomeric films is demonstrated on an indium tin oxide (ITO) electrode followed by an ITO top contact deposition yielding large-scale (junction area = 0.7 × 0.7 cm) two terminal molecular junctions. The molecular junctions exhibit non-volatile resistive switching at a relatively lower operational voltage, ±1 V, high ON/OFF electrical current ratio (≈10), low-energy consumption (SET/RESET = 27.94/14400 nJ), good cyclic stability (>300 cycles), and switching speed (SET/RESET = 25 ms/20 ms). A computational study suggests that accessible frontier molecular orbitals of metal-complex to the Fermi level of ITO electrodes facilitate charge transport at a relatively lower bias followed by a filamentformation. An extensive analysis is performed of the performance of binary neural networks exploiting the current-voltage features of the devices as binary synaptic weights and exploring their potential for neuromorphic logic-in-memory implementation of IMPLICATION (IMPLY) operation which can realize universal gates. The comprehensive analysis indicates that the proposed redox-active complex-based memory device may be a promising candidate for high-density data storage, energy-efficient implementation of neuromorphic networks with software-level accuracy, and logic-in-memory implementations.