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Design of terpolymers via copolymerization has emerged as a potential strategy for expanding the family of high-performing donor polymers and boosting the photovoltaic performance of non-fullerene polymer solar cells (PSCs). Herein, double-ester-substituted thiophenes and thienothiophenes are incorporated as third building blocks into the donor polymer PBDB-TF, developing two groups of terpolymers with donor-acceptor 1-donor-acceptor 2 (D-A1-D-A2)-type backbones. An optimum 10% concentration of double-ester-substituted thiophene units in PBDB-TF-T10 downshifts the molecular energy and increases the dielectric constant, and delivers proper miscibility and nanostructure in blends with the high-performing acceptor Y6. These characteristics are designed to synergistically enhance the photovoltage, photocurrent, and efficiency of PSCs. The resulting power conversion efficiency (PCE) of 16.4% surpasses the conventional PBDB-TF/Y6 PSCs, and it is among the best-performing PSCs based on PBDB-TF-derived terpolymers. Gratifyingly, PBDB-TF-T10 does not show significant batch-to-batch variation and it retains high PCEs above 16% in a broad range of molecular weights. This work introduces a facile strategy to easily synthesize terpolymers in combination with Y6 for the attainment of high-performing and reproducible non-fullerene PSCs.

Among the diverse nonfullerene acceptors, perylene bisimides (PBIs) have been attracting much attention due to their excellent electron mobility and tunable molecular and electronic properties by simply engineering the bay and head linkages. Herein, guided by two efficient small molecular acceptors, we designed, synthesized, and characterized a new nonfullerene small molecule PPDI with fine-tailored alkyl chains. Notably, a certificated PCE of 5.40% is realized in a simple structured fullerene-free polymer solar cell comprising PPDI as the electron acceptor and a fine-tailored 2D-conjugated polymer PBDT-TS1 as the electron donor. Moreover, the device behavior, morphological feature, and origin of high efficiency in PBDT-TS1/PPDI-based fullerene-free PSC were investigated. The synchronous selection and design of donor and acceptor materials reported here offer a feasible strategy for realizing highly efficient fullerene-free organic photovoltaics.