Pre‐Buried Additive for Cross‐Layer Modification in Flexible Perovskite Solar Cells with Efficiency Exceeding 22%

Halide perovskites have shown superior potentials in flexible photovoltaics due to their soft and high power-to-weight nature. However, interfacial residual stress and lattice mismatch due to the large deformation of flexible substrates have greatly limited the performance of flexible perovskite solar cells (F-PSCs). Here, ammonium formate (HCOONH₄ ) is used as a pre-buried additive in electron transport layer (ETL) to realize a bottom-up infiltration process for an in situ, integral modification of ETL, perovskite layer, and their interface. The HCOONH₄ treatment leads to an enhanced electron extraction in ETL, relaxed residual strain and micro-strain in perovskite film, along with reduced defect densities within these layers. As a result, a top power conversion efficiency of 22.37% and a certified 21.9% on F-PSCs are achieved, representing the highest performance reported so far. This work links the critical connection between multilayer mechanics/defect profiles of ETL-perovskite structure and device performance, thus providing meaningful scientific direction to further narrowing the efficiency gap between F-PSCs and rigid-substrate counterparts.