Fluorine-Induced Highly Reproducible Resistive Switching Performance: Facile Morphology Control through the Transition between J- and H-Aggregation

Improving the reproducibility and air-endurance of organic resistance switching (RS) devices, in particular multilevel-cell RS devices, is critical for the confirmation of its competency to realize big data storage capability. However, such enhancement still remains challenging. In this report, we demonstrated that fluorine (F)-embedding should be an effective way to enhance the overall performance of RS devices. Four new azo-cored analogues (IDAZO, FIDAZO, F₂IDAZO, and F₄IDAZO) have been designed and synthesized. These four compounds have similar structures with different numbers of F substituents. Interestingly, UV-vis measurements reveal that upon F-embedding, an exceptional transition from molecular J-aggregation to H-aggregation is achieved. As a result, the morphology of RS films becomes more and more uniform, as determined by AFM and XRD. Meanwhile, the hydrophobicity of RS film is promoted, which further improves the device atmospheric stability. The total RS reproducibility increases to 96% (the uppermost value), and the tristage RS reproducibility rises to 64%, accompanied by a more stable OFF state and lower logic SET voltages. Our study suggests F-embedding would be a promising strategy to achieve highly reproducible and air-endurable organic multilevel-cell RS devices.