Tin-based perovskite solar cells (Sn-PSCs) have emerged as promising environmentally viable photovoltaic technologies, but still suffer from severe non-radiative recombination loss due to the presence of abundant deep-level defects in the perovskite film and under-optimized carrier dynamics throughout the device. Herein, we healed the structural imperfections of Sn perovskites in an "inside-out" manner by incorporating a new class of biocompatible chelating agent with multidentate claws, namely, 2-Guanidinoacetic acid (GAA), which passivated a variety of deep-level Snrelated and I-related defects, cooperatively reinforced the passivation efficacy, released the lattice strain, improved the structural toughness, and promoted the carrier transport of Sn perovskites. Encouragingly, an efficiency of 13.7 % with a small voltage deficit of � 0.47 V has been achieved for the GAA-modified Sn-PSCs. GAA modification also extended the lifespan of Sn-PSCs over 1200 hours.

The quality of wide-band-gap (WBG) perovskite films plays an important role in tandem solar cells. Therefore, it is necessary to improve the performance of WBG perovskite films for the development of tandem solar cells. Here, we employ F-type pseudo-halogen additives (PF6 – or BF4 –) into perovskite precursors. The perovskite films with F-type pseudo-halogen additives have a larger grain size and higher crystal quality with lower defect density. At the same time, the perovskite lattice increases due to substitution of F-type pseudo-halogen anions for I–/Br–, and the stress distortion in the film is released, which effectively suppresses the recombination of carriers, reduces the charge transfer loss, and inhibits the phase separation. Finally, the power conversion efficiency (PCE) of the inverted 1.67 eV perovskite devices is significantly improved to over 20% with an impressive fill factor of 84.02% and excellent device stability. In addition, the PCE of the four-terminal (4T) perovskite/silicon tandem solar cells reached 27.35% (PF6 –) and 27.11% (BF4 –), respectively. This provides important guidance for further improving WBG perovskite solar cell performance.

No abstract

Mixed‐cation, small band‐gap perovskites via rationally alloying formamidinium (FA) and methylammonium (MA) together have been widely employed for blade‐coated perovskite solar cells with satisfied efficiencies. One of the stringent challenges lies in difficult control of the nucleation and crystallization kinetics of the perovskites with mixed ingredients. Herein, a pre‐seeding strategy by mixing FAPbI3 solution with pre‐synthesized MAPbI3 microcrystals has been developed to smartly decouple the nucleation and crystallization process. As a result, the time window of initialized crystallization has been greatly extended by 3 folds (i.e. from 5 s to 20 s), which enables the formation of uniform and homogeneous alloyed‐FAMA perovskite films with designated stoichiometric ratios. The resultant blade‐coated solar cells achieved a champion efficiency of 24.31 % accompanied by outstanding reproducibility with more than 87 % of the devices showing efficiencies higher than 23 %.

The high density of defects in MAPbI3 perovskite films brings about severe carrier nonradiative recombination loss, which lowers the performance of MAPbI3-based perovskite solar cells (PSCs). Here, methylamine cyanate (MAOCN) molecules were introduced into MAPbI3 solutions to manipulate the crystallizatsion of the MAPbI3 films. MAOCN molecules can slow down the volatilization rate of the solvent and delay the crystallization process of the MAPbI3 film. The crystal quality of the MAPbI3 films is effectively optimized without an additive residue. Perovskite films treated by MAOCN have lower defect density and longer carrier lifetime, which lowers the carrier recombination loss. Meanwhile, the MAPbI3 film based on MAOCN has a more hydrophobic surface. The final MAPbI3-based device efficiency reached 21.28% (V OC = 1.126 V, J SC = 23.29 mA/cm2, and FF = 81.13). After 30 days of storage under atmospheric conditions, the efficiency of unencapsulated MAOCN-based PSCs only dropped by about 5%.