Abstract
Transition-metal doping in perovskite nanocrystals strongly alters the photophysical properties of these nanocrystals. However, the details of the underlying thermal and optical processes within such an intriguing symmetry-breaking nanosystem are far from clear. Herein, we study the sensitively temperature-dependent and highly competent delocalized exciton and transition-metal ion-captured carrier recombination processes in manganese-doped CsPbBr0.6Cl2.4 nanocrystals. The combined experimental and theoretical studies reveal that both the exciton ionization and capture of the band-edge carriers by the manganese ions play the dominant roles in determining the proportion of the manganese ions-dominated recombination process. A density functional theory calculation of the temporal fluctuation of the manganese ions-accommodated localized orbitals further confirms that the thermally enhanced nonadiabatic electron-phonon coupling promotes the probability of the carrier localization. These findings reveal the respective crucial roles of the exciton ionization and carrier capture in the localized recombination process in the transition-metal-doped semiconductor nanocrystals.
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