Unraveling exciton–phonon coupling in individual FAPbI3 nanocrystals emitting near-infrared single photons

Ming Fu, Philippe Tamarat, Jean-Baptiste Trebbia, Maryna I. Bodnarchuk, Maksym V. Kovalenko, Jacky Even and Brahim Lounis ()
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Ming Fu: LP2N
Philippe Tamarat: LP2N
Jean-Baptiste Trebbia: LP2N
Maryna I. Bodnarchuk: Empa-Swiss Federal Laboratories for Materials Science and Technology
Maksym V. Kovalenko: Empa-Swiss Federal Laboratories for Materials Science and Technology
Jacky Even: Institut FOTON - UMR 6082
Brahim Lounis: LP2N

Nature Communications, 2018, vol. 9, issue 1, 1-10

Abstract: Abstract Formamidinium lead iodide (FAPbI3) exhibits the narrowest bandgap energy among lead halide perovskites, thus playing a pivotal role for the development of photovoltaics and near-infrared classical or quantum light sources. Here, we unveil the fundamental properties of FAPbI3 by spectroscopic investigations of nanocrystals of this material at the single-particle level. We show that these nanocrystals deliver near-infrared single photons suitable for quantum communication. Moreover, the low temperature photoluminescence spectra of FAPbI3 nanocrystals reveal the optical phonon modes responsible for the emission line broadening with temperature and a vanishing exciton–acoustic phonon interaction in these soft materials. The photoluminescence decays are governed by thermal mixing between fine structure states, with a two-optical phonon Raman scattering process. These results point to a strong Frölich interaction and to a phonon glass character that weakens the interactions of charge carriers with acoustic phonons and thus impacts their relaxation and mobility in these perovskites.

Date: 2018
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DOI: 10.1038/s41467-018-05876-0

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