Ultrathin Graphene Intercalation in PEDOT:PSS/Colorless Polyimide-Based Transparent Electrodes for Enhancement of Optoelectronic Performance and Operational Stability of Organic Devices

A novel flexible transparent electrode (TE) having a trilayer-stacked geometry and high optoelectronic performance and operational stability was fabricated by the spin coating method. The trilayer was composed of an ultrathin graphene (Gr) film sandwiched between a transparent and colorless polyimide (TCPI) layer and a methanesulfonic acid (MSA)-treated poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) layer containing dimethylsulfoxide and Zonyl fluorosurfactant (designated as MSA-PDZ film). The introduction of solution-processable TCPI enabled the direct formation of high-quality graphene on organic surfaces with a clean interface. Stable doping of graphene with the MSA-PDZ film enabled tuning of the inherent work function and optoelectronic properties of the PEDOT:PSS films, leading to a high figure of merit of ∼70 in the as-fabricated TEs. Particularly, from multivariate and repetitive harsh environmental tests (T = −50 to 90 °C, over 90 RH%), the TCPI/Gr heterostructure exhibited ex...