Energy and Charge Transfer Dynamics in Red-Emitting Hybrid Organo-Inorganic Mixed Halide Perovskite Nanocrystals

We report time-resolved spectral properties of highly stable and efficient red-emitting hybrid perovskite nanocrystals with the composition FA0.5MA0.5PbBr0.5I2.5 (FAMA PeNC) synthesized by using the hot-addition method. The PL spectrum of the FAMA PeNC shows a broad asymmetric band covering 580 to 760 nm with a peak at 690 nm which can be deconvoluted into two bands corresponding to the MA and FA domains. The interactions between the MA and FA domains are shown to affect the relaxation dynamics of the PeNCs from the subpicosecond to tens of nanoseconds scale. Time-correlated single-photon counting (TCSPC), femtosecond PL optical gating (FOG), and femtosecond transient absorption spectral (TAS) techniques were employed to study the intercrystal energy transfer (photon recycling) and intracrystal charge transfer processes between the MA and the FA domains of the crystals. These two processes are shown to increase the radiative lifetimes for the PLQYs exceeding 80%, which may play a key role in enhancing the performance of PeNC-based solar cells.