Insight into the exciton fine structure, the role of phonons and depolarization effects in halide perovskite nanocrystals
jacky even a, philippe tamarat b, philipe bourges c, guido roma d, claudine katan e, maryna bodnarchuk f, maksym kovalenko g, brahim lounis b
a Univ Rennes, INSA Rennes, CNRS, Institut FOTON - UMR 6082, F-35000 Rennes, France
b LP2N - Institut d'Optique, Université de Bordeaux & CNRS, 33400 Talence, Francia, Talence, France
c Université Paris-Saclay, CNRS, CEA, Laboratoire Léon Brillouin, Rue Joliot Curie, 3, Gif-sur-Yvette, France
d Université Paris-Saclay, CEA, Service de Recherches de Metallurgie Physique, Rue Joliot Curie, 3, Gif-sur-Yvette, France
e Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) - UMR 6226, F-35000 Rennes, France
f Laboratory for Thin Films and Photovoltaics, Empa − Swiss Federal Laboratories for Materials Science and Technology, Ueberlandstrasse, 129, Dübendorf, Switzerland
g Institute of Inorganic Chemistry, ETH Zürich, Zürich, Switzerland, Zurich, Switzerland
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting 2021 (NFM21)
#PerNC21. Perovskites II: Synthesis, Characterization, and Properties of Colloidal
Online, Spain, 2021 October 18th - 22nd
Organizers: Maksym Kovalenko, Ivan Infante and Lea Nienhaus
Invited Speaker, jacky even, presentation 216
DOI: https://doi.org/10.29363/nanoge.nfm.2021.216
Publication date: 23rd September 2021

Halide perovskite nanocrystals have been introduced in 2015 as a promising route to efficient light emitting devices, and more recently as potential single photon emitters. Their radiative recombinations are governed by excitons, but the bright or dark character of the ground state is debated. A Rashba effect correlated with a local polarization was proposed in 2018 as a general mechanism for inversion of bright and dark level ordering, but direct spectroscopic signatures of the dark exciton emission in the low-temperature photoluminescence of single FAPbBr3 and CsPbI3 nanocrystals under magnetic fields rather yield a dark singlet below the bright triplet. The dark-bright splitting values are in fair agreement with numerical estimations of the long-range electron–hole exchange interaction. The intense luminescence of perovskite nanocrystals is alternatively attributed to a reduced bright-to-dark phonon-assisted relaxation. The phonon side bands in nanocrystals match neutron scattering phonon spectroscopy results obtained at low temperature. Finally, a recent classification of 3D perovskites into ferroelectric or hyperferroelectric materials, points toward the role of the depolarization effect for the reduction of a spontaneous polarization in nanocrystals.

 

 

The research leading to these results has received funding from the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the grant agreement No 899141. (POLLOC).

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