Publication date: 28th August 2024
Tin-halide perovskites are deemed as a more sustainable alternative to lead-halide perovskites. However, a clear understanding and control of their chemistry remains slender compared to the lead counterparts in bulk and nano owing to their inability to provide a stable oxidation state (+2) to maintain a pristine crystal structure phase in ambient conditions. Being ionic, halide-perovskites (ASnX3) exhibit dimensional dynamics depending on the size of the intercalated cation (A+). Thus, it becomes important to develop a rational chemical design for directing the reaction towards a desired 3D or 2D perovskite structure. Our investigations uncover that a sub-stoichiometric amount of ligands and a high concentration of SnX2 salt are paramount to achieving stable, tunable, and monodisperse CsSnX3 perovskite nanocrystals (X – I, Br) with defined optical features. Pertaining to their comparable formation energies, the 2D perovskite phase ([R-NH3]2SnX4) can be easily converted to 3D nanocrystals via a cation exchange reaction in solution as well as in thin-films, and can undergo facile anion exchange reactions with benzoyl halides. The ligand coordination effects in the formation of FASnI3 nanocrystals reveal the presence of [SnI3]- complex as an intermediate species to form perovskite nanostructures. Finally, we demonstrate the hybrid organic-inorganic encapsulation by depositing a thin layer of PMMA followed by a 40 nm alumina layer via ALD improves the ambient stability of CsSnX3 NCs thin-film for up to record 15 days, to help facilitate their photophysical studies. This research highlights the insistent necessity for a comprehensive understanding of the synthesis and photophysical properties of tin-halide perovskite nanostructures to unlock their full potential.
This work was financially supported by the Dutch Research Council (NWO) via VENI grant number VI.Veni.192.048 and by the Advanced Materials research program of the Zernike National Research Centre under the Bonus Incentive Scheme of the Dutch Ministry for Education, Culture and Science.
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