Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.081
Publication date: 22nd December 2022
Perovskite nanocrystal superlattices are three-dimensional solid-state ordered ensembles of monodispersed semiconductor nanoparticles. Upon interaction with light pulses, these highly ordered systems can give rise to unexpected phenomena such as superfluorescence, a recently reported many-body quantum state in which the excitons generated in each single perovskite nanocrystal are coherently locked [1]. The possibility to realize macroscopic quantum states with high exciton densities, low energy broadening and long dephasing time, makes these systems promising platform to develop entangled multi-photon quantum light devices or quantum information storage systems [2, 3]. Among the halide perovskite nanocrystals, hybrid organic-inorganic compositions have attracted attention owing to high conversion efficiencies in solar cells [4] and the promise to maintain quantum coherence [5, 6]. For further progress in this field, relationship between cooperative phenomena, nanocrystal composition and excitonic features still need to be established.
In this work, we compare all-inorganic CsPbX3 (X = Cl, Br or I) and hybrid FAPbX3 (FA = formamidinium; X = Br or I) superlattices assembled from nanocrystals derived from either a direct synthesis or an aging-assisted size-selection. By combining halides and A-cation alloying, we demonstrate exciton tunability over all the visible spectrum. We employ an ultrashort resonant optical pumping scheme to study the collective states that can arise from an ordered system of quantum confined excitons interacting with laser pulses. Starting from superlattices of CsPbBr3 nanocrystals, we demonstrate that these systems can be driven across different quantum phases by tuning the laser intensity: from the excitonic Mott insulating phase to the collective superradiant state and the metallic electron-hole liquid phase. The behavior of CsPbBr3 is compared with that of FAPbI3 nanocrystal superlattices to understand structure-property relationships.
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