Vacuum-Assisted Thermal Annealing of CH₃NH₃PbI₃for Highly Stable and Efficient Perovskite Solar Cells

Solar cells incorporating lead halide-based perovskite absorbers can exhibit impressive power conversion efficiencies (PCEs), recently surpassing 15%. Despite rapid developments, achieving precise control over the morphologies of the perovskite films (minimizing pore formation) and enhanced stability and reproducibility of the devices remain challenging, both of which are necessary for further advancements. Here we demonstrate vacuum-assisted thermal annealing as an effective means for controlling the composition and morphology of the CH(3)NH(3)PbI(3) films formed from the precursors of PbCl(2) and CH(3)NH(3)I. We identify the critical role played by the byproduct of CH(3)NH(3)Cl on the formation and the photovoltaic performance of the perovskite film. By completely removing the byproduct through our vacuum-assisted thermal annealing approach, we are able to produce pure, pore-free planar CH(3)NH(3)PbI(3) films with high PCE reaching 14.5% in solar cell device. Importantly, the removal of CH(3)NH(3)Cl significantly improves the device stability and reproducibility with a standard deviation of only 0.92% in PCE as well as strongly reducing the photocurrent hysteresis.