The optimized exploitation of perovskite nanocrystals and nanoplatelets as highly efficient light sources requires a detailed understanding of the energy spacing within the exciton manifold. Dark exciton states are particularly relevant because they represent a channel that reduces radiative efficiency. Here, we apply large in -plane magnetic fields to brighten optically inactive states of CsPbBr3-based nanoplatelets for the first time. This approach allows us to access the dark states and directly determine the dark-bright splitting, which reaches 22 meV for the thinnest nanoplatelets. The splitting is significantly less for thicker nanoplatelets due to reduced exciton confinement. Additionally, the form of the magneto-PL spectrum suggests that dark and bright state populations are nonthermalized, which is indicative of a phonon bottleneck in the exciton relaxation process.
Thickness-dependent dark-bright exciton splitting and phonon bottleneck in CsPbBr3-based nanoplatelets revealed via magneto- optical spectroscopy / Wang, Sl; Dyksik, M; Lampe, C; Gramlich, M; Maude, Dk; Baranowski, M; Urban, As; Plochocka, P; Surrente, A. - In: NANO LETTERS. - ISSN 1530-6984. - 22:17(2022), pp. 7011-7019. [10.1021/acs.nanolett.2c01826]
Thickness-dependent dark-bright exciton splitting and phonon bottleneck in CsPbBr3-based nanoplatelets revealed via magneto- optical spectroscopy
Surrente, A
2022
Abstract
The optimized exploitation of perovskite nanocrystals and nanoplatelets as highly efficient light sources requires a detailed understanding of the energy spacing within the exciton manifold. Dark exciton states are particularly relevant because they represent a channel that reduces radiative efficiency. Here, we apply large in -plane magnetic fields to brighten optically inactive states of CsPbBr3-based nanoplatelets for the first time. This approach allows us to access the dark states and directly determine the dark-bright splitting, which reaches 22 meV for the thinnest nanoplatelets. The splitting is significantly less for thicker nanoplatelets due to reduced exciton confinement. Additionally, the form of the magneto-PL spectrum suggests that dark and bright state populations are nonthermalized, which is indicative of a phonon bottleneck in the exciton relaxation process.File | Dimensione | Formato | |
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