Diketopyrrolopyrrole-based terpolymers with tunable broad band absorption for fullerene and fullerene-free polymer solar cells

A series of random terpolymers with donor-acceptor-donor-acceptor molecular configuration, comprising fluorinated benzotriazole (FTAZ) and thienothiophene-capped diketopyrrolopyrrole (TTDPP) as the first and second electron-accepting moieties and thienyl-substituted benzodithiophene (BDTT) as the electron-donating unit, are designed for polymer solar cells. By tuning the ratio of TTDPP and FTAZ, the optoelectronic properties of the terpolymers are systematically varied. All materials exhibit a broad absorption window spanning from 300 to 900 nm, illustrating the success of the terpolymer approach. Fullerene-based polymer solar cells fabricated from the terpolymer with the highest content of TTDPP afford a power conversion efficiency of 5.7%, with a short-circuit current density of 15.2 mA cm -2. On the other hand, solar cell devices composed of the terpolymer with the lowest content of TTDPP and the narrow gap non-fullerene acceptor IEICO-4F exhibit a higher efficiency of 6.3%, with an enhanced short-circuit current density of 17.5 mA cm -2, as a result of a better complementarity in the absorption of the donor and acceptor materials and well-balanced charge carrier mobilities. This efficiency represents the best value for fullerene-free polymer solar cells based on DPP-containing polymers to date.