Mechanically Resilientand Highly Efficient FlexiblePerovskite Solar Cells with Octylammonium Acetate for Surface Adhesionand Stress Relief

Flexible perovskite solar cells (FPSCs) have advanced significantly because of their excellent power-per-weight performance and affordable manufacturing costs. The unsatisfactory efficiency and mechanical stability of FPSCs are bottleneck challenges that limit their application. Here, we explore the use of octylammonium acetate (OAAc) with a long, intrinsic, flexible molecular chain on perovskite films for surface adhesion and mechanical releasing. The results showed that OAAc with high structural flexibility and strong molecular interactions can act as a mechanical release layer in releasing residual tensile stress, confirmed by the film and device characterizations as well as finite-element simulation. Moreover, the passivation of the OAAc could increase the formation energy of defects including I vacancy, Pb vacancy, and Pb–I antisite. The experimental results showed that the trap states of perovskites were significantly suppressed after OAAc modification, which is beneficial to the construction of high-quality films. With a high open-circuit voltage of 1.196 V, the efficiency of the OAAc-treated devices increased from 23.14% to 25.47% on a rigid substrate (23.12% on a flexible substrate), yielding superior long-term and mechanical durability. The corresponding flexible device retains 74% of the initial value even after 8000 bending cycles at a bending radius of 5 mm.