Single-Emitter Spectra from an Ensemble

TL;DR

SPICEE is a novel spectrally filtered photon-correlation method that accurately recovers single-emitter spectra from ensemble measurements, enabling high-throughput analysis of nanoscale emitters' heterogeneity.

Contribution

The paper introduces SPICEE, a new technique combining spectral filtering and photon correlation to extract single-emitter spectra from ensemble data.

Findings

SPICEE accurately recovers single-emitter spectra from ensembles.

Application to ZnSeTe nanocrystals reveals subpopulations with distinct emission.

Ensemble spectral broadening is mainly due to a small subpopulation with different emission mechanisms.

Abstract

The heterogeneity in nanoscale emitters hinders efforts to understand their basic photophysics and limits their use in practical applications. Existing methods have difficulty accurately characterizing single-emitter spectra and optical heterogeneity on a statistical scale. Here, we introduce SPICEE (SPectrally Imbalanced Correlations from Ensemble Emission), a spectrally filtered photon-correlation technique that recovers single-particle emission lineshapes from an ensemble sample. Analytical derivations, numerical modeling, and experiments on a solution ensemble of emitters validate the technique. We apply SPICEE to blue-emitting ZnSeTe semiconductor nanocrystals relevant to display applications and find that the low color purity in the ensemble spectrum is primarily caused by a small subpopulation of nanocrystals with a distinct emission mechanism. This work demonstrates that SPICEE is a powerful high-throughput tool for accurately characterizing the single-emitter properties of nanoscale systems.