High efficiency and nonhalogenated solvent processing are important issues for commercial application of all-polymer solar cells (all-PSCs). In this regard, we increased the photovoltaic performance of all-PSCs to a benchmark power conversion efficiency (PCE) of 11.66% by manipulating the pre-aggregation of a new π-conjugated polymer donor (Nap-SiBTz) using toluene as a solvent. This use of Nap-SiBTz enhanced the absorption coefficient (λ = 9.30 × 10 cm), increased charge carrier mobility, suppressed trap-assisted recombination, improved bulk heterojunction morphology, and resulted in high PCEs of all-PSCs with an active layer thickness of 200 nm. To overcome severe charge recombination and energy losses, a 1-phenylnapthalene additive was used to achieve a well-ordered microstructure and molecular packing that inherently improved the device performances. The resulting encapsulation-free devices exhibited good ambient and thermal stabilities. The results of this study augur well for the future of the roll-to-roll production of all-PSCs.
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