Here we report a solution-processing strategy to stabilize the perovskite-based heterostructure. Strong Pb–Cl and Pb–O bonds formed between a [CH(NH2)2]x[CH3NH3]1−xPb1+yI3 film with a Pb-rich surface and a chlorinated graphene oxide layer. The constructed heterostructure can selectively extract photogenerated charge carriers and impede the loss of decomposed components from soft perovskites, thereby reducing damage to the organic charge-transporting semiconductors. Perovskite solar cells with an aperture area of 1.02 square centimeters maintained 90% of their initial efficiency of 21% after operation at the maximum power point under AM1.5G solar light (100 milliwatts per square centimeter) at 60°C for 1000 hours. The stabilized output efficiency of the aged device was further certified by an accredited test center.

Inverted perovskite solar cells (IPSCs) have attracted great attention in recent years due to reliable operational stability, negligible hysteresis and low-temperature fabrication process. To accelerate its commercialization, the focus of...

Organic–inorganic hybrid perovskite solar cells (PSCs) are a promising photovoltaic technology that has rapidly developed in recent years. Nevertheless, a large number of ionic defects within perovskite absorber can serve as non‐radiative recombination center to limit the performance of PSCs. Here, organic donor‐π‐acceptor (D‐π‐A) molecules with different electron density distributions are employed to efficiently passivate the defects in the perovskite films. The X‐ray photoelectron spectroscopy (XPS) analysis shows that the strong electron donating N,N‐dibutylaminophenyl unit in a molecule causes an increase in the electron density of the passivation site that is a carboxylate group, resulting in better binding with the defects of under‐coordinated Pb2+ cations. Carrier lifetime in the perovskite films measured by the time‐resolved photoluminescence spectrum is also prolonged by an increase in donation ability of the D‐π‐A molecules. As a consequence, these benefits contribute to an increase of 80 mV in the open circuit voltage of the devices, enabling a maximum power conversion efficiency (PCE) of 20.43%, in comparison with PCE of 18.52% for the control device. The authors' findings provide a novel strategy for efficient defect passivation in the perovskite solar cells based on controlling the electronic configuration of passivation molecules.

All‐inorganic cesium lead iodide perovskites (CsPbI3) are promising wide‐bandgap materials for use in the perovskite/silicon tandem solar cells, but they easily undergo a phase transition from a cubic black phase to an orthorhombic yellow phase under ambient conditions. It is shown that this phase transition is triggered by moisture that causes distortion of the corner‐sharing octahedral framework ([PbI6]4−). Here, a novel strategy to suppress the octahedral tilting of [PbI6]4− units in cubic CsPbI3 by systematically controlling the steric hindrance of surface organic terminal groups is provided. This steric hindrance effectively prevents the lattice distortion and thus increases the energy barrier for phase transition. This mechanism is verified by X‐ray diffraction measurements and density functional theory calculations. Meanwhile, the formation of an organic capping layer can also passivate the surface electronic trap states of perovskite absorber. These modifications contribute to a stable power conversion efficiency (PCE) of 13.2% for the inverted planar perovskite solar cells (PSCs), which is the highest efficiency achieved by the inverted‐structure inorganic PSCs. More importantly, the optimized devices retained 85% of their initial PCE after aging under ambient conditions for 30 days.

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