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Two poly(3-hexylthiophene) (P3HT) macromers containing a donor polymer with a polymerizable methacrylate (MA) end group, P3HT-CH₂-MA and P3HT-(CH₂)₂-MA, have been synthesized, and P3HT-(CH₂)₂-MA has been successfully homopolymerized and copolymerized with methyl methacrylate (MMA) into stereoregular brush polymers and graft copolymers, respectively, using chiral ansa -zirconocene catalysts. Macromer P3HT-CH₂-MA is too sterically hindered to polymerize by the current Zr catalysts, but macromer P3HT-(CH₂)₂-MA is readily polymerizable via either homopolymerization or copolymerization with MMA in a stereospecific fashion with both C ₂-ligated zirconocenium catalyst 1 and C  s -ligated zirconocenium catalyst 2 . Thus, highly isotactic (with mm % ≥ 92%) and syndiotactic (with rr % ≥ 93%) brush polymers, it -PMA- g -P3HT and st -PMA- g -P3HT, as well as well-defined stereoregular graft copolymers with different grafted P3HT densities, it -P(M)MA- g -P3HT and st -P(M)MA- g -P3HT, have been synthesized using this controlled coordination-addition polymerization system under ambient conditions. These stereoregular brush polymers and graft copolymers exhibit both thermal (glass and melting) transitions with T  g and T  m values corresponding to transitions within the stereoregular P(M)MA and crystalline P3HT domains. Acceptor molecules such as C 60 can be effectively encapsulated inside the helical cavity of st -P(M)MA- g -P3HT to form a unique supramolecular helical crystalline complex, thus offering a novel strategy to control the donor/acceptor solar cell domain morphology.

Stereoregular Brush Polymers and Graft Copolymers by Chiral Zirconocene-Mediated Coordination Polymerization of P3HT Macromers