Journal
CHEMISTRY OF MATERIALS
Volume 31, Issue 18, Pages 7761-7769Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.9b02944
Keywords
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Funding
- European Union [794560, 614897]
- Marie Curie Actions (MSCA) [794560] Funding Source: Marie Curie Actions (MSCA)
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A detailed investigation into the synthesis of green-emitting powders of Cs4PbBr6 and CsPbBr3 materials by antisolvent precipitation from CsBr-PbBr2 precursor solutions in dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) is reported. Various solvated lead bromide and polybromide species (PbBr2, [PbBr3](-), [PbBr4](2-), and possibly [PbBr5](3-) or [PbBr6](4-)) are detected in the precursor solutions by optical absorbance and emission spectroscopies. The solvodynamic size of the species in solution is strongly solvent-dependent: similar to 1 nm species were detected in DMSO, while significantly larger species were observed in DMF by dynamic light scattering. The solvodynamic size of the lead bromide species plays a critical role in determining the Cs-Pb-Br composition of the precipitated powders: smaller species favor the precipitation of Cs4PbBr6, while larger species template the formation of CsPbBr3 under identical experimental conditions. The powders have been characterized by Cs-133 and Pb-207 solid-state nuclear magnetic resonance, and Cs-133 sensitivity toward the different Cs environments within Cs4PbBr6 is demonstrated. Finally, the possible origins of green emission in Cs4PbBr6 samples are discussed. It is proposed that a two-dimensional Cs2PbBr4 inclusion may be responsible for green emission at similar to 520 nm in addition to the widely acknowledged CsPbBr3 impurity, although we found no conclusive experimental evidence supporting such claims.
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