Unveiling the Effect of Cooling Rate on Grown-in Defects Concentration in Polycrystalline Perovskite Films for Solar Cells with Improved Stability.

Numerous efforts are devoted to reducing the defects at perovskite surface and/or grain boundary; however, the grown-in defects inside grain is rarely studied. Here, the influence of cooling rate on the point defects concentration in polycrystalline perovskite film during heat treatment processing is investigated. With the combination of theoretical and experimental studies, this work reveals that the supersaturated point defects in perovskite films generate during the cooling process and its concentration improves as the cooling rate increases. The supersaturated point defects can be minimized through slowing the cooling rate. As a result, the optimized FAPbI3 polycrystalline films achieve a superior carrier lifetime of up to 12.6 µs and improved stability. The champion device delivers a 25.47% PCE (certified 24.7%) and retain 90% of their initial value after >1100 h of operation at the maximum power point. These results provide a fundamental understanding of the mechanisms of grown-in defects formation in polycrystalline perovskite film.

Inhibition of defect-induced α-to-δ phase transition for efficient and stable formamidinium perovskite solar cells.

Defects passivation is widely devoted to improving the performance of formamidinium lead triiodide perovskite solar cells; however, the effect of various defects on the α-phase stability is still unclear. Here, using density functional theory, we first reveal the degradation pathway of the formamidinium lead triiodide perovskite from α to δ phase and investigate the effect of various defects on the energy barrier of phase transition. The simulation results predict that iodine vacancies are most likely to trigger the degradation, since they obviously reduce the energy barrier of α-to-δ phase transition and have the lowest formation energies at the perovskite surface. A water-insoluble lead oxalate compact layer is introduced on the perovskite surface to largely suppress the α-phase collapse through hindering the iodine migration and volatilization. Furthermore, this strategy largely reduces the interfacial nonradiative recombination and boosts the efficiency of the solar cells to 25.39% (certified 24.92%). Unpackaged device can maintain 92% of its initial efficiency after operation at maximum power point under simulated air mass 1.5 G irradiation for 550 h.