| Abstract: | The long‐term performance and stability of perovskites are adversely affected by their porous microstructure, tensile residual stress, and electron transport kinetics. Here, a high‐speed pulsed laser processing technique is implemented to produce beneficial structural changes in organic–inorganic halide perovskites, including pore‐free, crystalline structure, reduced defects, and tensile residual stress. Moreover, halide perovskite films can be converted from p‐type to n‐type semiconductor, which originates from crystal structure changes, giving rise to carrier dynamic changes. Comparing with traditional thermal annealing, residual tensile stress of perovskite thin film decreases by 40% after pulse laser processing, which significantly increases its stability. Pulse‐laser‐induced thermomechanical shock momentum can create pore‐free perovskite thin films, contributing to much better reliability. Under humidity of 80% at room temperature for 500 h, the decomposition rate is reduced by more than two times, comparing thin films after pulsed laser processing with conventional thermal annealing. The thermal decomposition temperature of pulse‐laser‐processed perovskite thin film raises by 20 to about 220 °C. Pulse laser processing technique provides a scalable technique to tailor the structures in perovskite films with both temperature and loading control, further facilitates the design of perovskite‐based devices for service under harsh conditions, and also contributes to high‐performance optoelectronic applications. |
