Cooperative excitonic quantum ensemble in perovskite-assembly superlattice microcavities

Abstract

Perovskites-compounds with the CaTiO 3-type crystal structure-show outstanding performance in photovoltaics and multiparameter optical emitters due to their large oscillator strength, strong solar absorption, and excellent charge-transport properties. However, the ability to realize and control many-body quantum states in perovskites, which would extend their application from classical optoelectronic materials to ultrafast quantum operation, remains an open research topic. Here, we generate a cooperative quantum state of excitons in a quantum dot ensemble based on a lead halide perovskite, and we control the ultrafast radiation of excitonic quantum ensembles by introducing optical microcavites. The stimulated radiation of excitonic quantum ensemble in a superlattice microcavity is demonstrated to not be limited by the classical population-inversion condition, leading to a picosecond radiative duration time to dissipate all of the in-phase dipoles. Such a perovskite-assembly superlattice microcavity with a tunable radiation rate promises potential applications in ultrafast, photoelectric-compatible quantum processors.

Optical studies of semiconductor perovskite nanocrystals for classical optoelectronic applications and quantum information technologies: a review

“…However, if an ensemble of optical emitters can interact coherently via a common light field, their correlated emission dipoles would give rise to short and intense bursts of light [see Meanwhile, it might be feasible to embed perovskite NCs inside an optical cavity for the construction of superfluorescent lasers already achieved in atomic systems, 116,117 wherein the cooperative exciton recombination can result in an instant consumption of all coherent emission dipoles. In a recent attempt by Zhou et al, 114 the individual superlattices made of CsPbBr 3 NCs could be assembled again to form the microcavity with a quality factor of ∼1800. The occurrence of superfluorescence lasing could be deduced from the pumping-density dependences of the PL peaks and intensities shown in Figs.…”

A Highly Ordered Quantum Dot Supramolecular Assembly Exhibiting Photoinduced Emission Enhancement

“…Owing to the high dispersibility of QDs, most studies using QDs have been focused on the photophysical properties under single conditions, such as dispersed QDs in solution [14, 15] and single QD levels [16–19] . On the other hand, understanding the physical properties derived from inter‐QD interactions observed in the solid condition of QDs is quite important for the development of QD‐based materials science [20–23] . Although QD structures could be formed on substrates by the evaporation of solvents, such an assembly method gives rise to the formation of inhomogeneous and ill‐defined structures, and furthermore, the formation of assembled QDs in solution is quite difficult [24] .…”

Monodisperse Long-Chain Sulfobetaine-Capped CsPbBr3 Nanocrystals and Their Superfluorescent Assemblies

“…CsPbX 3 NC superlattices have recently triggered interest due to the emergence of collective light-emission phenomena, namely, superfluorescence (SF). 58 , 77 Specifically, at cryogenic temperatures—given the high oscillator strength of the transitions, low energetic disorder, and long exciton coherence time—these NCs undergo cooperative emission, which results in a red-shifted band with strongly accelerated radiative rates. Similarly, we find such superfluorescent emission also in supercystals of zwitterion-capped NCs ( Figure 5 ).…”