In flexible neuromorphic systems for realizing artificial intelligence, organic memristors are essential building blocks as artificial synapses to perform the information processing and memory. Despite much effort to implement artificial...

We demonstrate the physical pictures of the localization of the conductive filaments (CFs) growth in flexible electrochemical metallization (ECM) memristors through an interfacial triggering (IT) into the polymer electrolyte. The IT sites (ITSs), capable of controlling the pathways of the CF growth, are formed at the electrode–polymer interfaces via the Ostwald ripening at low temperatures (below 230 °C). The injection and migration of metal ions and the resultant CF growth are found to be effectively controlled through the ITSs with the local electric field enhancement. The reliability, uniformity, and switching voltage of the device are much improved by the presence of the ITSs. Our flexible ECM memristor exhibits a high mechanical flexibility and a stable memory performance under repeated bending deformations.

In this study, we propose an effective strategy for achieving the flexible one organic transistor–one organic memristor (1T–1R) synapse using the multifunctional organic memristor. The dynamics of the conductive nanofilament (CF) in a hydrophobic fluoropolymer medium is explored and a hydrophobic fluoropolymer-based organic memristor is developed. The flexible 1T–1R synapse can be fabricated using the solution process because the hydrophobic fluorinated polymer layer is produced on the organic transistor without degradation of the underlying semiconductor. The developed flexible synapse exhibits multilevel conductance with high reliability and stability because of the fluoropolymer film, which acts as a medium for CF growth and an encapsulating layer for the organic transistor. Moreover, the synapse cell shows potential for high-density memory systems and practical neural networks. This effective concept for developing practical flexible neural networks would be a basic platform to realize the smart wearable electronics.

Herein, the underlying mechanisms for the growth of conductive filaments (CFs) at a metal–polymer electrolyte interface through ion migration in organic electrochemical metallization (ECM) memristor are presented. It is observed that the free volume of voids (nanopores) in the polymer electrolyte serves as the pathways of metal‐cations whereas the interfacial topography between an active electrode and a polymer electrolyte determines the nucleation sites of the CFs. The growth kinetics of the CFs and the resultant resistive memory are found to vary with the molecular weight of the polymer electrolyte and the metal protrusions at the interface. Our direct observations show that the free volume of voids of the polymer electrolyte, varied with the molecular weight, dictates the ion transport for the growth and the disruption of the CFs. Our organic ECM‐based memristor with a hetero‐electrolyte exhibits high mechanical flexibility, low switching voltages reduced by about three times compared to those of conventional devices, and stable memory retention for longer than 104 s under repeated cycles of bending.

In flexible neuromorphic electronics, solution‐processed organic memristors are important elements to perform memory functions. Despite considerable development for improving performances of organic memristors, the devices still exhibit the poor reliability and uniformity due to the stochastic characteristics of the conductive filament (CF) growth. Herein, the effective concept of introducing the interfacial load polymer (ILP) layers that control the CF growth in flexible organic memristors is demonstrated. In the flexible organic memristor, the ILP serves as an internal load resistor that regulates the CF growth in the electrolyte medium and the electron blocking layer, hence realizing self‐rectifying characteristics. In particular, the ILP provides the self‐compliance current of the device, which delicately limits the overgrowth of CFs. The flexible device delivers higher electrical performance (better reliability, uniformity, and the switching currents) than conventional devices without the ILP. Moreover, the device operates stably under repeated bending–straightening deformations. This unprecedented concept of achieving the capabilities of self‐compliance current and self‐rectifying property in a single memristor will provide a practical platform for constructing and realizing next‐generation flexible neuromorphic systems.