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The buried interface has important effect on carrier extraction and nonradiative recombination of perovksite solar cells (PSCs). Herein, to inactivate the buried interfacial defects of perovskite and boost the crystallization quality of perovskite film, 3‐amino‐1‐adamantanol (AAD) serves as a pre‐buried interface modifier on nickel oxide (NiOx) surface to regulate the nucleation and crystallization process of perovskite precursor. The amino and hydroxyl groups in AAD molecule can synchronously coordinate with nickel ion (Ni3+) in NiOx and lead ion in perovskite, respectively. The dual action favors the ordered arrangement of AAD molecules between NiOx and perovskite, which not only enhances hole extraction in hole transport layer, but also provides active sites for homogeneous nucleation. Furthermore, AAD modifier blocks the unfavorable reaction between Ni3+ and perovskite, and effectively passivates the buried interfacial defects. The optimal inverted PSCs achieve a champion power conversion efficiency of 22.21% with negligible hysteresis, favorable thermal, optical, and long‐term stability. Thus, this strategy of modulating perovskite nucleation and crystallization by pre‐buried modifier is feasible for achieving efficient and stable inverted perovskite solar cells. [ABSTRACT FROM AUTHOR]

Lead‐free 2D antimony‐based halide perovskites with excellent optoelectronic properties, low toxicity, and good intrinsic stability are promising for photovoltaic devices. However, the power conversion efficiency (PCE) of antimony‐based perovskite solar cells (PSCs) is still lower than 3% due to the poor crystallinity and random orientation. Herein, it is found that the Cs3Sb2ClxI9‐x films prepared by adding methylamine chloride as an additive to the precursor solution can form a mixed intermediate phase with 0D dimer phase and 2D layered phase after low pressure treatment. During the annealing process, the 0D dimer phase will completely transition to 2D layered phase due to the partial replacement of I by Cl. Compared to adding SbCl3 directly, this method considerably increases the crystallinity of Cs3Sb2IxCl9‐x films. The obtained films have a preferential orientation along the (201) direction, which is beneficial for charge carrier transportation. Consequently, the champion device shows a PCE of 3.2%, which is one of the highest efficiencies achieved for inorganic Sb‐based PSCs with the n‐i‐p architecture to date. [ABSTRACT FROM AUTHOR]

Tin‐based halide perovskites attract incremental attention due to the favorable optoelectronic properties and ideal bandgaps. However, the poor crystalline quality is still the biggest challenge for further progress in tin‐based perovskite solar cells (PVSCs) due to the unfavorable defects and uncontrollable crystallization kinetics. Here, acetic acid (HAc) is first introduced to reduce the supersaturated concentration of the precursor solution to preferentially form pre‐nucleation clusters, thus inducing rapid nucleation for effective regulation of crystallization kinetics. In particular, the hydrogen ion and acetate ion contained in HAc can effectively inhibit the oxidation of Sn2+, and the hydrogen bonding interaction between HAc and iodide ion (I‐) greatly reduces the loss of I‐, which guarantees the I‐/Sn2+ stoichiometric ratio of the corresponding perovskite film close to theoretical value, thus effectively reducing the defect density and maintaining the perfect crystal lattice. Consequently, the HAc‐assisted tin‐based PVSCs achieve a champion power conversion efficiency of 12.26% with superior open‐circuit voltage up to 0.75 V. Moreover, the unencapsulated device maintains nearly 90% of the initial PCE even after 3000 h storage in nitrogen atmosphere. This demonstrated strategy enables to prepare high‐quality tin‐based perovskite film with lower defect density and lattice distortion. [ABSTRACT FROM AUTHOR]

Tin‐based halide perovskites attract incremental attention due to the favorable optoelectronic properties and ideal bandgaps. However, the poor crystalline quality is still the biggest challenge for further progress in tin‐based perovskite solar cells (PVSCs) due to the unfavorable defects and uncontrollable crystallization kinetics. Here, acetic acid (HAc) is first introduced to reduce the supersaturated concentration of the precursor solution to preferentially form pre‐nucleation clusters, thus inducing rapid nucleation for effective regulation of crystallization kinetics. In particular, the hydrogen ion and acetate ion contained in HAc can effectively inhibit the oxidation of Sn2+, and the hydrogen bonding interaction between HAc and iodide ion (I‐) greatly reduces the loss of I‐, which guarantees the I‐/Sn2+ stoichiometric ratio of the corresponding perovskite film close to theoretical value, thus effectively reducing the defect density and maintaining the perfect crystal lattice. Consequently, the HAc‐assisted tin‐based PVSCs achieve a champion power conversion efficiency of 12.26% with superior open‐circuit voltage up to 0.75 V. Moreover, the unencapsulated device maintains nearly 90% of the initial PCE even after 3000 h storage in nitrogen atmosphere. This demonstrated strategy enables to prepare high‐quality tin‐based perovskite film with lower defect density and lattice distortion. [ABSTRACT FROM AUTHOR]