Publication date: 3rd July 2020
Assemblies of lead halide perovskite nanocrystals are promising quantum emitters due to the electronic coupling and collective emission of nanocrystals, which reveal themselves through spectroscopic observables such as low energy narrow photoluminescence peaks and accelerated radiative decays. In order to bring these intriguing phenomena closer towards applications, it is crucial to understand how the stability of notoriously unstable lead halide perovskites affects them. Surprisingly, we found that similar spectroscopic features could arise due to the nanocrystal reactivity with the environment under the common sample storage conditions such as under vacuum or in air. The optical response of individual CsPbBr3 nanocube assemblies was studied with steady-state and time-resolved micro-photoluminescence techniques. The observed changes at T = 4 K include the appearance of low energy narrow emission peaks (with redshifts as large as ~105 meV and fwhm <20 meV) with lifetimes of ~10-40 ps, a nearly an order of magnitude faster than those of pristine assemblies. These results point to the reactivity of CsPbBr3 nanocrystals with themselves and their environment as a significant roadblock for studies of cooperative emission and highlight the need to develop strategies of lead halide perovskite nanocrystal stabilization which are compatible with high-quality self-assembly.
The work of D.B. was supported by the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement No. 794560 (RETAIN).
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