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Precursor Chemistry of Lead Bromide Perovskite Nanocrystals.
Dahl, Jakob C; Curling, Ethan B; Loipersberger, Matthias; Calvin, Jason J; Head-Gordon, Martin; Chan, Emory M; Alivisatos, A Paul.
Afiliación
  • Dahl JC; Department of Chemistry, University of California, Berkeley, California 94720, United States.
  • Curling EB; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
  • Loipersberger M; Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
  • Calvin JJ; Department of Chemistry, University of California, Berkeley, California 94720, United States.
  • Head-Gordon M; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
  • Chan EM; Department of Chemistry, University of California, Berkeley, California 94720, United States.
  • Alivisatos AP; Department of Chemistry, University of California, Berkeley, California 94720, United States.
ACS Nano ; 18(33): 22208-22219, 2024 Aug 20.
Article en En | MEDLINE | ID: mdl-39115283
ABSTRACT
We investigate the early stages of cesium lead bromide perovskite formation through absorption spectroscopy of stopped-flow reactions, high-throughput mapping, and direct synthesis and titration of potential precursor species. Calorimetric and spectroscopic measurements of lead bromide complex titrations combined with theoretical calculations suggest that bromide complexes with higher coordination numbers than previously considered for nonpolar systems can better explain observed behaviors. Synthesis mapping of binary lead halides reveals multiple lead bromide species with absorption peaks higher than 300 nm, including a previously observed species with a peak at 313 nm and two species with peaks at 345 and 370 nm that also appear as reaction intermediates during the formation of lead bromide perovskites. Based on theoretical calculations of excitonic energies that match within 50 meV, we give a preliminary assignment of these species as two-dimensional magic-sized clusters with side lengths of 2, 3, and 4 unit cells. Kinetic measurements of the conversion of benzoyl bromide precursor are connected to stopped-flow measurements of product formation and demonstrate that the formation of complexes and magic-sized clusters (i.e., nucleation) is controlled by precursor decomposition, whereas the growth rate of 2D and 3D perovskites is significantly slower.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Nano Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Nano Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos