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Abstract Fast reaction between organic salt and lead iodide always leads to small perovskite crystallites and concentrated defects. Here, polyacrylic acid is blended with organic salt, so as to regulate the crystallization in a two‐step growth method. It is observed that addition of polyacrylic acid retards aggregation and crystallization behavior of the organic salt, and slows down the reaction rate between organic salt and PbI 2 , by which “slow‐release effect” is defined. Such effect improves crystallization of perovskite. X‐ray diffraction study shows that, after addition of 2 m m polyacrylic acid, average crystallite size of perovskite increases from ≈40 to ≈90 nm, meanwhile, grain size increases. Thermal admittance spectroscopy study shows that trap density is reduced by nearly one order (especially for deep energy levels). Due to the improved crystallization and reduced trap density, charge recombination is obviously reduced, while lifetime of charge carriers in perovskite film and devices are prolonged, according to time‐resolved photoluminescence and transient photo‐voltage decay curve tests, respectively. Accordingly, power conversion efficiency of the device is promoted from 19.96 (±0.41)% to 21.84 (±0.25)% (with a champion efficiency of 22.31%), and further elevated to 24.19% after surface modification by octylammonium iodide. 

Hydrophobic and long-chain molecule oleylamine is used to modify the spiro-OMeTAD matrix, which is then adopted for the hole-transport layer in perovskite solar cells. It is observed that after moderate doping, the power conversion efficiency of the devices increases from 17.82 (±1.47)% to 20.68 (±0.77)%, with the optimized efficiency of 21.57% (AM 1.5G, 100 mW/cm2). The improved efficiency is ascribed to the favored charge extraction and retarded charge recombination, as reflected by transient photovoltage/photocurrent curves and impedance spectroscopy measurement. In addition, the grazing incidence photoluminescence spectrum reveals that oleylamine doping causes a blue shift of the luminescence peak of the surface layer of the halide perovskite film, while the Mott−Schottky study observes 100 mV increment in the built-in potential, both of which indicate possible defect passivation behavior on the perovskite. Moreover, an accelerated damp test observes that moisture resistance of the device is also upgraded, which is due to the improved hydrophobicity of the spiro-OMeTAD matrix. 

Capsaicin is used to modify SnO 2 quantum dots and then used as an electron-transfer material for perovskite solar cells. After capsaicin modification, the power conversion efficiency of the devices increases from 19.90 (± 0.47)% to 21.87 (± 0.28)% with a champion device of 22.24% (AM 1.5G, 100 mW/cm 2 ). Transient photovoltage and photocurrent decay show that, after the capsaicin doping, the lifetime increases from 21.55 (± 1.54) to 27.63 (± 1.45)  μs, while the charge extraction time reduces from 1.90 (± 0.09) to 1.67 (± 0.06)  μs. Time-resolved photoluminescence and impedance spectrum studies show similar results. The accelerated charge transfer and retarded recombination are due to defect passivation. Space charge limited current study shows that, after modification, the trap density of devices is reduced from 2.24 × 10 15 to 1.28 × 10 15  cm −3 . X-ray photoelectron spectroscopy and theoretical calculation indicate that the reduced trap density is due to the chemical interaction between carbonyl group (from capsaicin) and Sn atom, and that between carbonyl group and Pb atom.