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All‐inorganic cesium lead halide flexible perovskite solar cells (f‐PSCs) exhibit superior thermal stability compared to their organic‐inorganic hybrid counterparts. However, their flexibility and efficiency are still below‐par for practical viability. This study presents an approach involving the introduction of multifunctional molecule ammonium benzenesulfonate (ABS) to selectively etch 0D‐Cs4Pb(IBr)6 from the mixed‐dimensional perovskite film surface, to attain more contact area between the perovskite and hole transport layer for improved hole extraction and transport. It is found that the ABS molecules bind to the perovskite lattice surface via O atoms and NH4+, effectively passivating surface defects and enhancing phase stability. The hydrophobic nature of the benzene ring in ABS further contributes to operational stability, leading to high cell efficiency of 15.00%, accompanied by enhanced operational stability. Even after undergoing 60 000 flexing cycles at a curvature radius of 5 mm, the ABS‐treated f‐PSC still retains over 98.5% of its initial efficiency. This multifunctional strategy for modifying typical mixed‐dimensional perovskite compositions significantly enhances the photovoltaic performance and stability of flexible all‐inorganic f‐PSCs. [ABSTRACT FROM AUTHOR]

The mechanical durability and efficiency of all‐inorganic flexible perovskite solar cells (f‐PSCs) still require enhancement for practical applications. In this study, a creative debridement strategy to improve the mechanical durability and photovoltaic performance of all‐inorganic f‐PSCs by pre‐bending the flexible perovskite film and then depositing the passivation agent 2‐mercaptopyridine is proposed. The pre‐bending process induced the generation of microcracks in the perovskite film surface, and 2‐mercaptopyridine can more effectively penetrate the interior of the film through the microcracks, thereby further passivating deep surface defects. These microcracks and defects can be perfectly repaired by 2‐mercaptopyridine. Bidentate coordination sites of S and N in 2‐mercaptopyridine show stronger binding energy with surface defects. The debridement strategy effectively enhanced the crystallization of the film surface and markedly inhibited crack propagation during the film's bending process. The optimized device achieves a champion power conversion efficiency (PCE) of 14.74%. The pre‐bent and passivated all‐inorganic f‐PSC shows 104% of its initial PCE after 15 000 bending cycles at a curvature radius of 3 mm. Remarkably, even after undergoing 70 000 bending cycles at a curvature radius of 5 mm, pre‐bent, and passivated f‐PSC can retain over 93% of its initial PCE, exhibiting excellent mechanical durability. [ABSTRACT FROM AUTHOR]

All-inorganic CsPbI 3 films necessitate higher annealing temperatures for high-quality crystallization. Consequently, the conventional low-temperature solution approach often results in poor crystallization in flexible CsPbI 3 films, significantly degrading the optoelectronic performance and stability of flexible perovskite solar cells (f-PSCs). Herein, a heterogeneous CaF 2 nanocrystal seed-induced strategy has been successfully utilized to achieve enhanced crystallization of a flexible CsPbI 2.81 Br 0.19 film. Due to their good lattice match with the perovskite material, CaF 2 nanoparticles can decrease the critical Gibbs free energy of CsPbI 2.81 Br 0.19 perovskite nucleation, thereby accelerating γ-phase CsPbI 2.81 Br 0.19 crystallization at low temperatures. This leads to an improved crystalline quality of the flexible perovskite film at low temperatures, which minimizes defects and enhances the stability of f-PSCs. The CsPbI 2.81 Br 0.19 f-PSCs achieved a champion power conversion efficiency of 15.03% and demonstrated mechanical stability, retaining 98.1% of their initial efficiency even after 60 000 bending cycles with a curvature radius of 5 mm.

The anti-solvent-free fabrication of high-efficiency perovskite solar cells (PSCs) holds immense significance for the transition from laboratory-scale to large-scale commercial applications. However, the device performance is severely hindered by the increased occurrence of surface defects resulting from the lack of control over nucleation and crystallization of perovskite using anti-solvent methods. In this study, 2-(naphthalen-2-yl)ethylamine hydriodide (NEAI) is employed as the surface passivator for perovskite films without using any anti-solvent. Naphthalene demonstrates strong π-π conjugation, which aids in the efficient extraction of charge carriers. Additionally, the naphthalene-ring moieties form a tight attachment to the perovskite surface. After NEAI treatment, FA and I vacancies are selectively occupied by NEA + and I - in NEAI respectively, thus effectively passivating the surface defects and isolating the surface from moisture. Ultimately, the optimized NEAI-treated device achieves a promising power conversion efficiency (PCE) of 24.19% (with a certified efficiency of 23.94%), featuring a high fill factor of 83.53%. It stands out as one of the reported high PCEs achieved for PSCs using the spin-coating technique without the need for any anti-solvent so far. Furthermore, the NEAI-treated device can maintain ≈87% of its initial PCE after 2000 h in ambient air with a relative humidity of 30% ± 5%., (© 2024 Wiley‐VCH GmbH.)