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The poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)with well-matched work function and conductivity as interfacial layer and electrode for polymer solar cells(PSCs)was optimized by sulfonate poly(aryl ether sulfone)(SPES),sulfonated carbon nanotubes(S-CNTs),sulfonated graphene(S-Gra),and carbon nanotubes(CNTs).