Quantifying the Distribution of Biexciton Emission Efficiencies in Colloidal Quantum Shells

Abstract

The efficiency of multi-photon emission is an important characteristic of quantum light sources. Bright multi-photon emission is desirable for high-power lighting and lasers, while its complete suppression is required for high-purity single-photon generation. In colloidal quantum emitters, multi-photon emission can vary significantly between individual particles. Resolving this heterogeneity remains challenging with conventional particle-by-particle approaches. Here, we introduce a crosstalk-suppressed SPAD-array photon-correlation approach for high-throughput quantification of multi-photon emission from more than 1000 colloidal quantum shells. By projecting two images of the same sample onto distant regions of the detector array, we avoid short-range crosstalk between detector pixels. Time gating suppresses dark-count coincidences and distinguishes individual emitters from clusters. Applying this method to quantum shells reveals a near-Gaussian distribution of biexciton emission efficiencies, with a mean of 0.55 and an estimated intrinsic standard deviation of 0.12. Intra-batch correlations between the biexciton efficiency and the particle brightness are consistent with the volume scaling of Auger quenching. These results establish SPAD-array photon correlation as a scalable route to resolve multi-photon heterogeneities in nanoparticle ensembles.