Impact of processing conditions on the film formation of lead-free halide double perovskite Cs2AgBiBr6

Lead-free halide double perovskites with enhanced stability have gained attention as a promising environmentally friendly alternative to lead-based halide perovskites. Amongst different halide double perovskites, Cs2AgBiBr6 has shown attractive optoelectronic properties and stability, making it a promising candidate for stable high-efficiency optoelectronic devices. Motivated by a data mining effort, we present here the effects of different processing strategies on the microstructure and thin-film formation dynamics of Cs2AgBiBr6. We apply some of the most successfully used solvent engineering approaches from the halide perovskite research to halide double perovskites, namely antisolvent- and additive-assisted synthesis. Using in situ spectroscopy and diffraction, the film formation of Cs2AgBiBr6 is investigated during spin coating, and the subsequent post-deposition thermal annealing. Dropping antisolvents during spin coating induces immediate supersaturation and crystallization of the wet film, whereas the time of dropping the antisolvent has implications on the film formation dynamics and the final microstructure. For additive (HBr)-assisted synthesis, we show how the addition of HBr affects colloid formation in solution and thus influences the crystallization pathway during thin-film processing. Finally, HBr additive simplifies synthesis in that it doesn't require solution and substrate preheating to obtain pinhole-free films even with higher thickness.

Automated summary

Lead-free halide double perovskites, specifically Cs2AgBiBr6, have shown promising optoelectronic properties and stability. In this study, different processing strategies, such as antisolvent- and additive-assisted synthesis, were applied to investigate the microstructure and thin-film formation dynamics of Cs2AgBiBr6. Dropping antisolvents during spin coating promoted immediate supersaturation and crystallization of the wet film, while the timing of antisolvent addition affected film formation dynamics and final microstructure. Additive (HBr)-assisted synthesis influenced colloid formation in solution and influenced the crystallization pathway during thin-film processing. HBr additive simplified the synthesis process and enabled the formation of pinhole-free films, even with increased thickness.