Abstract
Perovskites—compounds with the CaTiO3-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.
Highlights
Perovskites—compounds with the CaTiO3-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
Packed semiconductor quantum dots (QDs) superlattices with long-range order could offer a high density of exciton states, low energy broadening, and long dephasing time of particles, all of which enable the formation of macroscopic quantum states[12]
Transmission electron microscopy (TEM) and fast Fourier transform reveal that the CsPbBr3 QDs are cubic with very good crystallinity (Supplementary Fig. 2)
Summary
Perovskites—compounds with the CaTiO3-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. 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. We integrate the high quality of a QD superlattice and the optical controllability of a cavity in a perovskite microstructure (Fig. 2 and Supplementary Fig. 2) Such a highly symmetric, long-range-ordered perovskite QDSM could show both superfluorescence (SF) behavior and an optically stimulated amplification effect (i.e., lasing) above the critical excitation density. Cooperative excitons exhibit quantum behavior during their lasing process, in which the perovskite system consumes all the cooperative components of dipoles by the CESF channel, rather than being limited by the populationinversion condition, as in classical lasers (Fig. 4) By utilizing such a unique characteristic, the radiation time of cooperative exciton ensemble is shortened to be picoseconds
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