The Growth Dynamics of Organic–Inorganic Metal Halide Perovskite Films

Organic-inorganic metal halide perovskite films have emerged as potential candidate materials for photoelectric devices because of their superior optoelectronic properties. The performance of these devices depends on the quality of perovskite films defined by their grain size, crystallinity, and absence of pinholes. While solution-based processing is the most cost-effective and scalable approach to producing these films, the impact of the process parameters on the film quality and nanoscale details of these processes are unknown. Specifically, it is unclear how perovskites grow from a liquid precursor to form solid-phase nanocrystals and how these nanocrystals arrange to form a uniform film. Here, using liquid-phase transmission electron microscopy (TEM), we show how perovskite nanocrystals nucleate from a precursor solution and then grow and coalesce to form a polycrystalline film. Furthermore, we show how additives, such as urea, can improve the film crystallinity by increasing perovskite solubility, which induces the dissolution and subsequent redeposition of smaller crystals onto larger grains. Our approach to studying the growth of perovskite films provides an important insight into improving the synthesis of perovskites and other technologically relevant crystalline films.