Superfluorescent scintillation from coupled perovskite quantum dots

TL;DR

This paper reports the discovery of superfluorescence in coupled perovskite quantum dots under X-ray excitation, leading to significantly faster scintillation emission rates and potential improvements in detector technology.

Contribution

It demonstrates a novel collective emission phenomenon in perovskite quantum dots under X-ray excitation, surpassing the intrinsic spontaneous emission limit.

Findings

Achieved a 14-fold increase in emission rate with a 230 ps lifetime.

Observed spectral shifts and broader spectra under X-ray excitation.

Confirmed superfluorescence behavior using g^(2) measurements.

Abstract

Scintillation, the process of converting high-energy radiation to detectable visible light, is pivotal in advanced technologies spanning from medical diagnostics to fundamental scientific research. Despite significant advancements toward faster and more efficient scintillators, there remains a fundamental limit arising from the intrinsic properties of scintillating materials. The scintillation process culminates in spontaneous emission of visible light, which is restricted in rate by the oscillator strength of individual emission centers. Here, we observe a novel collective emission phenomenon under X-ray excitation, breaking this limit and accelerating the emission. Our observation reveals that strong interactions between simultaneously excited coupled perovskite quantum dots can create collective radioluminescence. This effect is characterized by a spectral shift and an enhanced rate of emission, with an average lifetime of 230 ps, 14 times faster than their room temperature spontaneous emission. It has been established that such quantum dots exhibit superfluorescence under UV excitation. However, X-ray superfluorescence is inherently different, as each high-energy photon creates multiple synchronized excitation events, triggered by a photoelectron and resulting in even faster emission rates, a larger spectral shift, and a broader spectrum. This observation is consistent with a quantum-optical analysis explaining both the UV-driven and X-ray-driven effects. We use a Hanbury-Brown-Twiss g^(2) ({\tau}) setup to analyze the temperature-dependent temporal response of these scintillators. Collective radioluminescence breaks the limit of scintillation lifetime based on spontaneous emission and could dramatically improve time-of-flight detector performance, introducing quantum enhancements to scintillation science.