Green-Emitting Powders of Zero-Dimensional Cs4PbBr6: Delineating the Intricacies of the Synthesis and the Origin of Photoluminescence
Articolo
Data di Pubblicazione:
2019
Citazione:
Green-Emitting Powders of Zero-Dimensional Cs4PbBr6: Delineating the Intricacies of the Synthesis and the Origin of Photoluminescence / A. Ray, D. Maggioni, D. Baranov, Z. Dang, M. Prato, Q.A. Akkerman, L. Goldoni, E. Caneva, L. Manna, A.L. Abdelhady. - In: CHEMISTRY OF MATERIALS. - ISSN 0897-4756. - 31:18(2019 Sep 24), pp. 7761-7769. [10.1021/acs.chemmater.9b02944]
Abstract:
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: ~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 133Cs and 207Pb solid-state nuclear magnetic
resonance and 133Cs 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 a green emission
at ~520 nm in addition to the widely acknowledged CsPbBr3 impurity, although we found no
conclusive experimental evidence supporting such claim.
Tipologia IRIS:
01 - Articolo su periodico
Elenco autori:
A. Ray, D. Maggioni, D. Baranov, Z. Dang, M. Prato, Q.A. Akkerman, L. Goldoni, E. Caneva, L. Manna, A.L. Abdelhady
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