Polythiophene-based terpolymers with modulated aggregation behaviors for high-performance organic solar cells with 16.6% efficiency

Polythiophenes (PTs) are an attractive class of polymer donors (PDs) for organic solar cells (OSCs) owing to their relatively simple structures and scalable synthesis. Herein, a series of chlorinated thiazole-incorporated PT terpolymers are designed and high-performance OSCs with a power conversion efficiency (PCE) of 16.6% are demonstrated. By incorporating two different units, 3,3 & PRIME;-difluoro-2,2 & PRIME;-bithiophene (T2F2) and thieno[3,2-b] thiophene (TT), the aggregation properties of the terpolymers (PTz-FX; X = 0, 30, 50, 70, and 100, where X represents the mole percentage of T2F2 to total T2F2 +TT) are modulated. Among the PTz-FX series, PTz-F70 is found to be the optimal PD because its suitably tuned aggregation property leads to an optimized blend morphology with well-developed crystalline structures and donor-acceptor intermixed domains. The balanced morphology not only promotes charge generation/transport but also suppresses charge recombination in OSC devices. Thus, the PTz-F70-based OSCs achieve the highest PCE (16.6%), outperforming the OSCs based on PTz-FX with extremely strong (PTz-F100, PCE= 14.7%) or weak (PTz-F0, PCE = 12.0%) aggregation properties. The PCE of the PTz-F70-based OSCs is one of the highest performances among PT-based binary OSCs. This study highlights the importance of controlling the aggregation property of PTs for achieving high-performance PT-based OSCs.

Automated summary

By designing a series of chlorinated thiazole-incorporated polythiophene terpolymers, the aggregation properties were modulated, leading to high-performance organic solar cells. Among the terpolymers, PTz-F70 showed the best performance with the highest power conversion efficiency. This study highlights the importance of controlling the aggregation property of polythiophenes for achieving high-performance polythiophene-based organic solar cells.