Black phosphorus quantum dots (BPQDs) are proposed as effective seed-like sites to modulate the nucleation and growth of CsPbI2Br perovskite crystalline thin layers, allowing an enhanced crystallization and remarkable morphological improvement. We reveal that the lone-pair electrons of BPQDs can induce strong binding between molecules of the CsPbI2Br precursor solution and phosphorus atoms stemming from the concomitant reduction in coulombic repulsion. The four-phase transition during the annealing process yields an α-phase CsPbI2Br stabilized by BPQDs. The BPQDS/CsPbI2Br core-shell structure concomitantly reinforces a stable CsPbI2Br crystallite and suppresses the oxidation of BPQDs. Consequently, a power conversion efficiency of 15.47% can be achieved for 0.7 wt % BPQDs embedded in CsPbI2Br film-based devices, with an enhanced cell stability, under ambient conditions. Our finding is a decisive step in the exploration of crystallization and phase stability that can lead to the realization of efficient and stable inorganic perovskite solar cells.

Today's state‐of‐the‐art perovskite solar cells (PSCs) are utilizing polycrystalline perovskite thin films via solution‐processing at low temperature (<150 °C). It is extremely significant to enlarge grain size and passivate trap states for perovskite thin films to achieve high power conversion efficiency. Herein, a strategy for defect passivation of perovskite films via metal ion Ni2+ is for the first time reported. It is found that addition of Ni2+ can significantly generate polyporous PbI2 films due to a different solubility between NiCl2 and PbI2 which benefits penetration of MAI and thus formation of large grain perovskite films eventually. It further demonstrated that Ni2+ ions can effectively passivate PbI3− antisite defects and restrain the generation of Pb0 by interacting with the under‐coordinated halide anions and halide‐rich antisites. Therefore, introducing moderate Ni2+ ions result in a significant increase in photoluminescence lifetime from 285 to 732 ns. Accordingly, a power conversion efficiency of 20.61% can be achieved for the 3% Ni2+ addition‐based PSCs with an enhanced cell stability under ambient conditions. This work provides a promising route toward perovskite films featuring with high crystallinity and low trap‐density.

Layered Ruddlesden−Popper (RP) phase perovskite compounds have emerged as promising photovoltaic materials for solar cell applications, but they suffer from poor absorption and strong exciton-binding energy. Herein, fluoro-, chloro-, and bromo-substitutions on the 4-position of the phenyl group in the component C 6 H 5 CH 2 CH 2 NH 3 + (PEA + ) are designed and synthesized to investigate their effect on the layered RP type H-PEA 2 MA 2 Pb 3 I 10 (MA = CH 3 NH 3 ) perovskite as an example. Single-crystal X-ray diffraction and temperature-dependent photoluminescence spectroscopy characterization reveal the electron-withdrawing halogen in organic cations decreases the distortion of inorganic sheets and significantly reduces the impact of two-dimensional quantum and dielectric confinement. This is further verified with an increased visible absorption and lower excitonbinding energy for these new layered RP-type perovskite compounds. A planar structured perovskite solar cell using an F-PEA 2 MA 2 Pb 3 I 10 layer achieves a power conversion efficiency of 5.8%, which is better than that of the reference H-PEA 2 MA 2 Pb 3 I 10 .