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Increase in incident light and surface modification of the charge transport layer are powerful routes to achieve high‐performance efficiency of perovskite solar cells (PSCs) by improving the short‐circuit current density (JSC) and charge transport characteristics, respectively. However, few techniques are studied to reduce reflection loss and simultaneously improve the electrical performance of the electron transport layer (ETL). Herein, an inclined fluorine (F) sputtering process to fabricate high‐performance PSCs is proposed. The proposed process simultaneously implements the antireflection effect of F coating and the effect of F doping on a TiO2 ETL, which increases the amount of light transmitted into the PSC due to the extremely low refractive index (≈1.39) and drastically improves the electrical properties of TiO2. Consequently, the JSC of the F coating and doping perovskite solar cell (F‐PSC) increased from 25.05 to 26.01 mA cm−2, and the power conversion efficiency increased from 24.17% to 25.30%. The unencapsulated F‐PSC exhibits enhanced air stability after 900 h of exposure to ambient environment atmosphere (30% relative humidity, 25 °C under dark condition). The inclined F sputtering process in this study can become a universal method for PSCs from the development stage to commercialization in the future. [ABSTRACT FROM AUTHOR]

Pb‐free Sn‐based perovskite solar cells (PSCs) have significant potential for application in photovoltaic devices because of their suitable bandgap, low exciton binding energy, high carrier mobility, and long diffusion length. However, their performance is hampered by several issues. Sn‐based perovskites are highly susceptible to oxidation, which induces a high concentration of defects and degrades the chemical stability of the perovskite crystals. Herein, the anion formate (HCOO−) can effectively suppress the oxidation of Sn in the pure formamidinium tin triiodide (FASnI3) perovskite without using A‐site cationic additives. Moreover, the presence of formate results in a uniform pinhole‐free perovskite film with a low trap density, reduced charge carrier recombination, and improved charge extraction. Density functional theory calculations show that formate‐treated FASnI3 has improved stability against oxidative Sn degradation. The formate‐treated PSC achieves a power conversion efficiency of 12.11% at a high open‐circuit voltage of 0.71 V. The device exhibits improved stability in ambient air in which it maintained over 80% of its initial power conversion efficiency after 180 min because oxidation is inhibited owing to the strong interaction between Sn and formate. [ABSTRACT FROM AUTHOR]