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.

Interfacial modification, which serves multiple roles, is vital for the fabrication of efficient and stable perovskite solar cells. Here, a multifunctional interfacial material, biguanide hydrochloride (BGCl), is introduced between tin oxide (SnO2) and perovskite to enhance electron extraction, as well as the crystal growth of the perovskite. The BGCl can chemically link to the SnO2 through Lewis coordination/electrostatic coupling and help to anchor the PbI2. Better energetic alignment, reduced interfacial defects, and homogeneous perovskite crystallites are achieved, yielding an impressive certified power conversion efficiency (PCE) of 24.4%, with an open‐circuit voltage of 1.19 V and a drastically improved fill factor of 82.4%. More importantly, the unencapsulated device maintains 95% of its initial PCE after aging for over 500 h at 20 °C and 30% relative humidity in ambient conditions. These results suggest that the incorporation of BGCl is a promising strategy to modify the interface and control the crystallization of the perovskite, toward the attainment of highly efficient and stable perovskite solar cells as well as other perovskite‐based electronics.

A highly flexible and durable transparent graphene electrode with thermal stability was developed via the direct integration of polyimide (PI) on graphene. Due to the high transparency of PI-integrated graphene electrode and intimate contact between graphene and PI substrate, high-efficiency flexible organic solar cell with a PCE of 15.2% and outstanding mechanical robustness was obtained.

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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.