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Synthetic Variation and Structural Trends in Layered Two-Dimensional Alkylammonium Lead Halide Perovskites
Name
Paritmongkol et al - 2D perovskite structure - ChemRxiv 2019.pdf
Description
Submitted version
Size
3.77 MB
Format
Adobe PDF
Checksum (MD5)
abbb9ee650209caf9b32fd6ed030d9b5
Author(s)
Paritmongkol, Watcharaphol
Dahod, Nabeel S
Stollmann, Alexia
Mao, Nannan
Settens, Charles
Zheng, Shao-Liang
Tisdale, William A
Date Issued
2019
Journal
Chemistry of Materials
Publisher
American Chemical Society (ACS)
Version
Original manuscript
Abstract
© 2019 American Chemical Society. We report the cooling-induced crystallization of layered two-dimensional (2D) lead halide perovskites with controllable inorganic quantum-well thicknesses (n = 1, 2, 3, and 4), organic-spacer chain lengths (butyl-, pentyl-, and hexylammonium), A-site cations (methylammonium and formamidinium), and halide anions (iodide and bromide). Using single-crystal X-ray diffraction, we refined crystal structures for the iodide family as a function of these compositional parameters and across their temperature-dependent phase transitions. In general, lower-symmetry crystal structures, increasing extents of organic-spacer interdigitation, and increasing organic-spacer corrugation tilts are observed at low temperature. Moreover, greater structural distortions are observed in lead halide octahedra closest to the organic-spacer layer, and higher-n structures exhibit periodic variation in Pb-I bond lengths. These structural trends are used to explain corresponding temperature-dependent changes in the photoluminescence spectra. We also provide detailed guidance regarding the combination of synthetic parameters needed to achieve phase-pure crystals of each composition and discuss difficulties encountered when trying to synthesize particular members of the 2D perovskite family containing formamidinium or cesium as the A-site cation. These results provide a foundation for understanding structural trends in 2D lead halide perovskites and the effects these trends have on their thermal, electronic, and optical properties.
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DOI of Published Version
10.1021/acs.chemmater.9b01318
