Controlling the nucleation and growth kinetics of lead halide perovskite quantum dots

Quinten Akkerman (1, 2) , Tan Nguyen (3) , Simon Boehme (1, 2) , Federico Montanarella (1, 2) , Dmitry Dirin (1, 4) , Philipp Wechsler (1) , Finn Beiglböck (2) , Gabriele Rainò (1, 2) , Rolf Erni (5, 2) , Claudine Katan (3) , Jacky Even (6) , Maksym Kovalenko (1, 2)

1 D-CHAB - Department of Chemistry and Applied Biosciences [ETH Zürich]
2 EMPA - Swiss Federal Laboratories for Materials Science and Technology [Dübendorf]
3 ISCR - Institut des Sciences Chimiques de Rennes
4 EMPA - Swiss Federal Laboratories for Materials Science and Technology [St Gallen]
5 Electron Microscopy Center
6 FOTON - Institut des Fonctions Optiques pour les Technologies de l'informatiON

Colloidal lead halide perovskite (LHP) nanocrystals are of interest as photoluminescent quantum dots (QDs) whose properties depend on the size and shape. They are normally synthesized on subsecond time scales through hard-to-control ionic metathesis reactions. We report a room-temperature synthesis of monodisperse, isolable spheroidal APbBr 3 QDs (A=Cs, formamidinium, methylammonium) that are size-tunable from 3 to over 13 nanometers. The kinetics of both nucleation and growth are temporally separated and drastically slowed down by the intricate equilibrium between the precursor (PbBr 2 ) and the A[PbBr 3 ] solute, with the latter serving as a monomer. QDs of all these compositions exhibit up to four excitonic transitions in their linear absorption spectra, and we demonstrate that the size-dependent confinement energy for all transitions is independent of the A-site cation.

Domaines: Chimie théorique et/ou physique

Quinten Akkerman, Tan Nguyen, Simon Boehme, Federico Montanarella, Dmitry Dirin, et al.. Controlling the nucleation and growth kinetics of lead halide perovskite quantum dots. Science, 2022, 377 (6613), pp.1406-1412. ⟨10.1126/science.abq3616⟩. ⟨hal-03773436⟩