DOI: https://doi.org/10.29363/nanoge.hpatom.2022.008
Publication date: 30th October 2021
To produce perovskite thin films with high device performances, various fabrication methodologies have been developed leading to thin films with different surface structures and crystal morphologies. Whilst tremendous efforts have been devoted to characterizing macro- and microscopic structures within these films to better understand the processing-property-performance relationship, the materials’ atomic structure and its influence on device performance remain poorly understood. Therefore, we employed pair distribution function (PDF) analysis of X-ray total scattering data to obtain crystallographic and compositional information of methylammonium-lead-iodide (MAPbI3) thin films[1].
We studied a series of MAPbI3 thin films prepared by the conventional antisolvent method and our recently developed new approach via flash infrared annealing (FIRA)[2]. Combining with the XRD data from the X-ray total scattering experiments, we identified two intermediate phases present in considerable quantities (> 30 wt%) and exhibiting very short structure coherence lengths (< 2 nm). These intermediates form sequentially upon annealing, adopting a 2D layered stacking arrangement, which seems to be structurally related to the PbI2 precursor and eventually transforms into the 3D perovskite at high temperatures. The presence of the intermediate(s) was observed in all samples, regardless of the thin-film preparation method. Further annealing results in a degradation of the thin film where both the intermediates and the perovskite decompose to PbI2. We also found that the presence of these intermediates and PbI2 is associated with a reduced power conversion efficiency, suggesting further improvement in film preparation to minimise these secondary phases is crucial to enhance the overall device performance.
This work offers critical insight into the perovskite formation pathway and highlights the advantage of total scattering as a promising modern technique to establish the important link between the short-range structures of the perovskite materials and their functionalities.
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