Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating

Shambhavi Pratap, Finn Babbe, Nicola S. Barchi, Zhenghao Yuan, Tina Luong, Zach Haber, Tze-Bin Song, Jonathan L. Slack, Camelia V. Stan, Nobumichi Tamura, Carolin M. Sutter-Fella () and Peter Müller-Buschbaum ()
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Shambhavi Pratap: Physik-Department, Lehrstuhl für Funktionelle Materialien, Technische Universität München
Finn Babbe: Chemical Sciences Division, Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Nicola S. Barchi: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Zhenghao Yuan: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Tina Luong: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Zach Haber: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Tze-Bin Song: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Jonathan L. Slack: Advanced Light Source, Lawrence Berkeley National Laboratory
Camelia V. Stan: Advanced Light Source, Lawrence Berkeley National Laboratory
Nobumichi Tamura: Advanced Light Source, Lawrence Berkeley National Laboratory
Carolin M. Sutter-Fella: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Peter Müller-Buschbaum: Physik-Department, Lehrstuhl für Funktionelle Materialien, Technische Universität München

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Complex phenomena are prevalent during the formation of materials, which affect their processing-structure-function relationships. Thin films of methylammonium lead iodide (CH3NH3PbI3, MAPI) are processed by spin coating, antisolvent drop, and annealing of colloidal precursors. The structure and properties of transient and stable phases formed during the process are reported, and the mechanistic insights of the underlying transitions are revealed by combining in situ data from grazing-incidence wide-angle X-ray scattering and photoluminescence spectroscopy. Here, we report the detailed insights on the embryonic stages of organic-inorganic perovskite formation. The physicochemical evolution during the conversion proceeds in four steps: i) An instant nucleation of polydisperse MAPI nanocrystals on antisolvent drop, ii) the instantaneous partial conversion of metastable nanocrystals into orthorhombic solvent-complex by cluster coalescence, iii) the thermal decomposition (dissolution) of the stable solvent-complex into plumboiodide fragments upon evaporation of solvent from the complex and iv) the formation (recrystallization) of cubic MAPI crystals in thin film.

Date: 2021
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DOI: 10.1038/s41467-021-25898-5

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