Ultra-narrow room-temperature emission from single CsPbBr<sub>3</sub> perovskite quantum dots.

Rainò, Gabriele; Yazdani, Nuri; Boehme, Simon C; Kober-Czerny, Manuel; Zhu, Chenglian; Krieg, Franziska; Rossell, Marta D; Erni, Rolf et al. · Nat Commun · 2022

basic_science · Level V

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Abstract

Semiconductor quantum dots have long been considered artificial atoms, but despite the overarching analogies in the strong energy-level quantization and the single-photon emission capability, their emission spectrum is far broader than typical atomic emission lines. Here, by using ab-initio molecular dynamics for simulating exciton-surface-phonon interactions in structurally dynamic CsPbBr<sub>3</sub> quantum dots, followed by single quantum dot optical spectroscopy, we demonstrate that emission line-broadening in these quantum dots is primarily governed by the coupling of excitons to low-energy surface phonons. Mild adjustments of the surface chemical composition allow for attaining much smaller emission linewidths of 35-65 meV (vs. initial values of 70-120 meV), which are on par with the best values known for structurally rigid, colloidal II-VI quantum dots (20-60 meV). Ultra-narrow emission at room-temperature is desired for conventional light-emitting devices and paramount for emerging quantum light sources.