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A detailed investigation into the synthesis of green-emitting powders of Cs 4 PbBr 6 and CsPbBr 3 materials by antisolvent precipitation from CsBr-PbBr 2 precursor solutions in dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) is reported. Various solvated lead bromide and polybromide species (PbBr 2 , [PbBr 3 ] - , [PbBr 4 ] 2- , and possibly [PbBr 5 ] 3- or [PbBr 6 ] 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: ~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 Cs 4 PbBr 6 , while larger species template the formation of CsPbBr 3 under identical experimental conditions. The powders have been characterized by 133 Cs and 207 Pb solid-state nuclear magnetic resonance, and 133 Cs sensitivity toward the different Cs environments within Cs 4 PbBr 6 is demonstrated. Finally, the possible origins of green emission in Cs 4 PbBr 6 samples are discussed. It is proposed that a two-dimensional Cs 2 PbBr 4 inclusion may be responsible for green emission at ~520 nm in addition to the widely acknowledged CsPbBr 3 impurity, although we found no conclusive experimental evidence supporting such claims.

chemistry of materials

Green-Emitting Powders of Zero-Dimensional Cs<sub>4</sub>PbBr<sub>6</sub>: Delineating the Intricacies of the Synthesis and the Origin of Photoluminescence

Green-Emitting Powders of Zero-Dimensional Cs4PbBr6: Delineating the Intricacies of the Synthesis and the Origin of Photoluminescence

Green-Emitting Powders of Zero-Dimensional Cs₄PbBr₆: Delineating the Intricacies of the Synthesis and the Origin of Photoluminescence