A combined molecular dynamics and experimental study of two-step process enabling low-temperature formation of phase-pure alpha-FAPbI(3)

P Ahlawat and A Hinderhofer and EA Alharbi and HZ Lu and A Ummadisingu and HY Niu and M Invernizzi and SM Zakeeruddin and MI Dar and F Schreiber and A Hagfeldt and M Gratzel and U Rothlisberger and M Parrinello, SCIENCE ADVANCES, 7, eabe3326 (2021).

DOI: 10.1126/sciadv.abe3326

It is well established that the lack of understanding the crystallization process in a two-step sequential deposition has a direct impact on efficiency, stability, and reproducibility of perovskite solar cells. Here, we try to understand the solid-solid phase transition occurring during the two-step sequential deposition of methylammonium lead iodide and formamidinium lead iodide. Using metadynamics, x-ray diffraction, and Raman spectroscopy, we reveal the microscopic details of this process. We find that the formation of perovskite proceeds through intermediate structures and report polymorphs found for methylammonium lead iodide and formamidinium lead iodide. From simulations, we discover a possible crystallization pathway for the highly efficient metastable alpha phase of formamidinium lead iodide. Guided by these simulations, we perform experiments that result in the low-temperature crystallization of phase-pure alpha-formamidinium lead iodide.

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