A new metric to control nucleation and grain size distribution in hybrid organic–inorganic perovskites by tuning the dielectric constant of the antisolvent
| Autor: | Joshua J. Choi, Paulette Clancy, Eric N. Holmgren, Blaire A. Sorenson, Lucy U. Yoon |
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| Rok vydání: | 2021 |
| Předmět: |
Materials science
Renewable Energy Sustainability and the Environment Nucleation Plumbate 02 engineering and technology General Chemistry Dielectric 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Grain size 0104 chemical sciences Solvent chemistry.chemical_compound Chemical engineering chemistry General Materials Science Density functional theory Thin film 0210 nano-technology Perovskite (structure) |
| Zdroj: | Journal of Materials Chemistry A. 9:3668-3676 |
| ISSN: | 2050-7496 2050-7488 |
| DOI: | 10.1039/d0ta12364a |
| Popis: | In perovskite research, there is a widely exploited but poorly explained phenomenon in which the addition of “antisolvents (ATS)” to precursor solutions results in higher-quality films. We explain the mechanism and driving force underlying an antisolvent-driven solvent extraction process. Density functional theory calculations uncover the defining effects of antisolvent choice on the extent of complexation between a lead salt and a methylammonium cation in solution. We experimentally validate the computational results using ultraviolet-visible spectroscopy and 207Pb nuclear magnetic spectroscopy of methylammonium lead iodide solutions, containing both a processing solvent and an antisolvent. Furthermore, we uncover, and subsequently identify, the appearance of new species in solution as a result of the addition of the antisolvent. We observe that the choice of antisolvent has a substantial effect on the nature of the complexation of the methylammonium lead iodide (MAPbI3) precursor species, whose origin we explain at an atomic level; specifically, the lower the dielectric of the antisolvent, the stronger the intermolecular binding energy between methylammonium cation (MA+) cation and PbI3− plumbate, independent of the solvent or antisolvent interaction with the lead salt. Thin films were characterized using scanning electron microscopy; images of the films show how the addition of an antisolvent influences and, importantly, can be used to alter thin-film grain size. Grain size and distribution in thin films is reflected by the choice of antisolvent, promoting slower nucleation rates, a lower nucleation density, and hence larger final grain size. |
| Databáze: | OpenAIRE |
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