Organic Solar Cells with Graphene Electrodes and Vapor Printed Poly(3,4-ethylenedioxythiophene) as the Hole Transporting Layers

For the successful integration of graphene as a transparent conducting electrode in organic solar cells, proper energy level alignment at the interface between the graphene and the adjacent organic layer is critical. The role of a hole transporting layer (HTL) thus becomes more significant due to the generally lower work function of graphene compared to ITO. A commonly used HTL material with ITO anodes is poly(3,4-ethylenedioxythiophene) (PEDOT) with poly(styrenesulfonate) (PSS) as the solid-state dopant. However, graphene's hydrophobic surface renders uniform coverage of PEDOT:PSS (aqueous solution) by spin-casting very challenging. Here, we introduce a novel, yet simple, vapor printing method for creating patterned HTL PEDOT layers directly onto the graphene surface. Vapor printing represents the implementation of shadow masking in combination with oxidative chemical vapor deposition (oCVD). The oCVD method was developed for the formation of blanket (i.e., unpatterened) layers of pure PEDOT (i.e., no PSS) with systematically variable work function. In the unmasked regions, vapor printing produces complete, uniform, smooth layers of pure PEDOT over graphene. Graphene electrodes were synthesized under low-pressure chemical vapor deposition (LPCVD) using a copper catalyst. The use of another electron donor material, tetraphenyldibenzoperiflanthene, instead of copper phthalocyanine in the organic solar cells also improves the power conversion efficiency. With the vapor printed HTL, the devices using graphene electrodes yield comparable performances to the ITO reference devices (η(p,LPCVD) = 3.01%, and η(p,ITO) = 3.20%).