Further improvement and stabilization of perovskite solar cell (PSC) performance are essential to achieve the commercial viability of next-generation photovoltaics. Considering the benefits of fluorination to conjugated materials for energy levels, hydrophobicity, and noncovalent interactions, two fluorinated isomeric analogs of the well-known hole-transporting material (HTM) Spiro-OMeTAD are developed and used as HTMs in PSCs. The structure–property relationship induced by constitutional isomerism is investigated through experimental, atomistic, and theoretical analyses, and the fabricated PSCs feature high efficiency up to 24.82% (certified at 24.64% with 0.3-volt voltage loss), along with long-term stability in wet conditions without encapsulation (87% efficiency retention after 500 hours). We also achieve an efficiency of 22.31% in the large-area cell.

A series of polymer acceptors PF2-DTC, PF2-DTSi, and PF2-DTGe with identical molecular backbone but different central bridging atoms in tricyclic-fused donor units were developed. In all-PSCs, the PF2-DTSi-based blend film exhibited excellent mechanical robustness with an impressively high PCE of up to 10.77%. Moreover, the flexible solar cell based on this blend retained >90% of its initial PCE after bending and relaxing 1,200 times at a bending radius of 4 mm.

Considering the potential applications of all-polymer solar cells (all-PSCs) as wearable power generators, there is an urgent need to develop photoactive layers that possess intrinsic mechanical endurance, while maintaining a high power-conversion efficiency (PCE).Herein a strategy is demonstrated to simultaneously control the intercalation behavior and nanocrystallite size in the polymer-polymer blend by using a newly developed, high-viscosity polymeric additive, poly(dimethylsiloxane-co-methyl phenethylsiloxane) (PDPS), into the TQ-F:N2200 all-PSC matrix. A mechanically robust 10wt% PDPS blend film with a great toughness was obtained. Our results provide a feasible route for producing high-performance ductile all-PSCs, which can potentially be used to realize stretchable all-PSCs as a linchpin of next-generation electronics.

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Considering the special functions of fused-ring aromatic building blocks and Si-atom in high-performance donor-acceptor-conjugated materials at the same time, herein the synthesis of a novel fused-ring tricyclic heterocycle, triisopropylsilyl-substituted benzo[1,2-b:4,5-c′]dithiophene-4,8-dione (iBDD-Si), an isomer of well-known benzo[1,2-c:4,5-c′]dithiophene-4,8-dione is presented. The iBDD-Si-based copolymer series (PM6, PM6-5Si, PM6-10Si, and PM6-15Si) is synthesized via Stille polymerization, revealing fine-tuned optical and electrochemical properties, and molecular packing with varying iBDD-Si contents in the backbone. Organic solar cells are fabricated by pairing the copolymer donors with nonfullerene acceptor N3 and characterized. High power conversion efficiency of more than 17% is achieved using the PM6-5Sibased solar cell, which is attributed to the balanced charge transport, enhanced charge generation/dissociation kinetics, and minimized total energy and recombination losses. It is demonstrated that iBDD-Si is a promising backbone toolbox for various high-performance conjugated materials.