Solvent-Free Method for Defect Reduction and Improved Performance of p-i-n Vapor-Deposited Perovskite Solar Cells

As perovskite-based photovoltaics near commercialization, it is imperative to develop industrial-scale defect-passivation techniques. Vapor deposition is a solvent-free fabrication technique that is widely implemented in industry and can be used to fabricate metal-halide perovskite thin films. We demonstrate markably improved growth and optoelectronic properties for vapor-deposited [CH(NH₂)₂]_0.83Cs_0.17PbI₃ perovskite solar cells by partially substituting PbI₂ for PbCl₂ as the inorganic precursor. We find the partial substitution of PbI₂ for PbCl₂ enhances photoluminescence lifetimes from 5.6 ns to over 100 ns, photoluminescence quantum yields by more than an order of magnitude, and charge-carrier mobility from 46 cm²/(V s) to 56 cm²/(V s). This results in improved solar-cell power conversion efficiency, from 16.4% to 19.3% for the devices employing perovskite films deposited with 20% substitution of PbI₂ for PbCl₂. Our method presents a scalable, dry, and solvent-free route to reducing nonradiative recombination centers and hence improving the performance of vapor-deposited metal-halide perovskite solar cells.