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Volatile A-cation halide (AX) additives such as formamidinium chloride and methylammonium chloride have been widely employed for high-efficiency perovskite solar cells (PSCs). However, it remains unstudied how they influence the perovskite film stoichiometry and the solar cell performance and operational stability. Hereby, our work shows that over annealing of formamidinium chloride-containing perovskite films leads to a Pb-rich surface, resulting in a high initial efficiency, which however decays during maximum power point tracking (MPPT). On the contrary, perovskite films obtained by a shorter annealing time at the same temperature provide good stability during MPPT but a lower initial efficiency. Thus, we deduce that an optimal annealing is vital for both high efficiency and operational stability, which is then confirmed in the case where methylammonium chloride additive is used. With optimized perovskite annealing conditions, we demonstrate efficient and stable p-i-n PSCs that show a best power conversion efficiency of 20.7% and remain 90% of the initial performance after a 200 h MPPT at 60 °C under simulated 1 sun illumination with high UV content. Our work presents a comprehensive understanding on how volatile AX impacts perovskite film stoichiometry and its correlation to the device performance and operational stability, providing a new guideline for fabricating high-efficiency and operationally stable PSCs.

Ion migration mechanisms are often behind degradation pathways in perovskite solar cells under operating conditions.

Volatile A-cation halide (AX) additives such as formamidinium chloride and methylammonium chloride have been widely employed for high-efficiency perovskite solar cells (PSCs). However, it remains unstudied how they influence the perovskite film stoichiometry and the solar cell performance and operational stability. Hereby, our work shows that over annealing of formamidinium chloride-containing perovskite films leads to a Pb-rich surface, resulting in a high initial efficiency, which however decays during maximum power point tracking (MPPT). On the contrary, perovskite films obtained by a shorter annealing time at the same temperature provide good stability during MPPT but a lower initial efficiency. Thus, we deduce that an optimal annealing is vital for both high efficiency and operational stability, which is then confirmed in the case where methylammonium chloride additive is used. With optimized perovskite annealing conditions, we demonstrate efficient and stable p–i–n PSCs that show a best power conversion efficiency of 20.7% and remain 90% of the initial performance after a 200 h MPPT at 60 °C under simulated 1 sun illumination with high UV content. Our work presents a comprehensive understanding on how volatile AX impacts perovskite film stoichiometry and its correlation to the device performance and operational stability, providing a new guideline for fabricating high-efficiency and operationally stable PSCs.

Perovskite solar cells have shown their potential for multijunction applications due to their tunable bandgap. This research focuses on triple cation (3C) wide bandgap perovskites ranging from 1.6 to 1.76 eV, an ideal bandgap choice for 2-terminal tandems. The bandgap is changed via the X-site substitution of iodine (I) with bromine (Br) and via cation substitution, with various concentrations of cesium (Cs), methylammonium (MA), and formamidinium (FA). As a result, it is seen that cation engineering is a viable solution to fine-tune the bandgap and prevent a photoinduced segregation. Moreover, a champion efficiency of 18.3% is reported with a 1.67 eV bandgap.

In few years, perovskite solar devices have reached high efficiency on lab scale cells. Upscaling to module size, effective perovskite recipe and posttreatment are of paramount importance to the breakthrough of the technology. Herein this work, the development of a low-temperature planar n-i-p perovskite module (11 cm(2) aperture area, 91% geometrical fill factor) is reported on, exploiting the defect passivation strategy to achieve an efficiency of 19.1% (2% losses stabilized) with near-zero hysteresis, that is the most unsolved issue in the perovskite photovoltaic technology. The I/Br (iodine/bromide) halide ion ratio of the triple-cation perovskite formulation and deposition procedure are optimized to move from small area to module device and to avoid the detrimental effect of dimethyl sulfoxide (DMSO) solvent. The organic halide salt phenethylammonium iodide (PEAI) is adopted as surface passivation material on module size to suppress perovskite defects. Finally, homogeneous and defect-free layers from cell to module with only 8% relative efficiency losses, high reproducibility, and optimized interconnections are scaled by laser ablation methods. The homogeneity of the perovskite layers and of the full stack was assessed by optical, morphological, and light beam-induced current (LBIC) mapping characterizations.