Building process design rules for microstructure control in wide-bandgap mixed halide perovskite solar cells by a high-throughput approach

Wide bandgap mixed halide perovskites ABX3, in which X can be I, Br, or Cl, are promising materials to form highly efficient optoelectronic devices, because the optical bandgap can be controlled over a wide range by variation of the halogen composition. However, significant nonradiative losses must be overcome to approach the efficiency limit of single-junction solar cells. Here, we present a high throughput-based investigation of the influence of processing parameters on nonradiative losses in the perovskite bulk. We perform antisolvent crystallization during spin coating and vary the solvent type, its volume, and the temperature of the subsequent annealing step. We use the photoluminescence quantum yield (PLQY) as a proxy to the presence of nonradiative losses and PL spectra as a qualitative probe for sample morphology. Using Gaussian process regression, we find that we can reliably predict PLQY from the PL spectral shape. This means that the PL spectral shape conveys the essential photophysics controlling PL quenching and thus nonradiative charge recombination. In comparison with scanning electron micrographs and x-ray diffraction data, we find that nonradiative losses in polycrystalline perovskite films are caused by increased domain size dispersion. Our method provides a simple and fast structure-sensitive in-line probe for fast morphology optimization in a high-throughput fashion.

Automated summary

A study was conducted on the influence of processing parameters on nonradiative losses in perovskite bulk, revealing the potential to control the photoluminescence quantum yield and optimize material morphology by varying the processing conditions. The research also found that nonradiative losses in polycrystalline perovskite films are attributed to increased domain size dispersion.