Exciton linewidth broadening induced by exciton-phonon interactions in CsPbBr3 nanocrystals.

Abstract

Quantum dephasing of excitonic transitions in CsPbBr3 nanocrystals has been studied using two-dimensional electronic spectroscopy at cryogenic temperatures. The exciton-phonon interactions for acoustic and optical modes exhibit different effects on the coherent dynamics of excitonic transitions. The homogeneous linewidth shows a proportional dependence on the temperature, suggesting the primary dephasing channel of the elastic scattering between exciton and acoustic modes. The exciton-optical mode interaction is manifested as the beatings of off-diagonal signals in the population time domain at the frequencies of 29 and 51cm-1, indicating phonon replicas of excitonic transitions arising from coherent exciton-phonon interaction. The insight information of exciton homogeneous broadening in perovskite nanocrystals is essential for the potential application of quantum light sources.