Transition between cooperative emission regimes in giant perovskite nanocrystals

TL;DR

This study explores how temperature and excitation density influence the transition between superfluorescence and amplified spontaneous emission in giant CsPbBr3 perovskite nanocrystals, revealing fundamental cooperative light emission mechanisms.

Contribution

It demonstrates the controllable transition between superfluorescence and ASE in perovskite nanocrystals, providing new insights into their cooperative emission regimes.

Findings

Superfluorescence observed below 45 K.

ASE dominates between 45 K and 100 K.

Temperature and excitation density control emission regimes.

Abstract

Interactions between emitters within an ensemble can give rise to cooperative processes that significantly alter the properties of the emitted light. One such process is superfluorescence (SF), where excited electric dipoles spontaneously couple coherently and effectively radiate as one macroscopic emitter. It requires low energetic disorder, high temporal coherence and oscillator strength, and sub-wavelength volumes of material can be sufficient. Conversely, amplified spontaneous emission (ASE) originates from an avalanche-like stimulated amplification of initially spontaneously emitted photons and does not necessitate temporally coherent interactions among the emitters, but rather requires spatially long enough light propagation within the material to harvest the optical gain. Cesium lead halide perovskite nanocrystals (NCs) are one of the very few materials where both ASE (in disordered films) and SF (in ordered assemblies) were observed, however leaving unclear whether and how these regimes could be connected. Here, we demonstrate that temperature and excitation density can drive the transition between both regimes in a thin film of giant CsPbBr3 perovskite NCs. At temperatures below 45 K, excitonic SF was observed, whereas above a transition range between 45 K and 100 K, ASE prevails, but requires increased optical excitation and emitter density. Our results work out the different collective effects present in lead halide perovskites, providing fundamental insights into cooperative phenomena and important guidance for the development of compact and bright (quantum) light sources.