Statistical analysis of photoluminescence decay kinetics in quantum dot ensembles: Effects of inorganic shell composition and environment

Abstract

Discerning the kinetics of photoluminescence (PL) decay of packed quantum dots (QDs) and QD-based hybrid materials is of crucial importance for achieving their promising potential. However, the interpretation of the decay kinetics of QD-based systems, which usually are not single-exponential, remains challenging. Here, we present a method for analyzing photoluminescence (PL) decay curves of fluorophores by studying their statistical moments. A certain combination of such moments, named as the n-th order moments' ratio, R n , is studied for several theoretical decay curves and experimental PL kinetics of CdSe quantum dots (QDs) acquired by time-correlated single photon counting (TCSPC). For the latter, three different case studies using the R n ratio analysis are presented, namely, (i) the effect of the inorganic shell composition and thickness of the core-shell QDs, (ii) QD systems with Förster resonance energy transfer (FRET) decay channels, and (iii) system of QDs near a layer of plasmonic nanoparticles. The proposed method is shown to be efficient for the detection of slight changes in the PL kinetics, being time-efficient and requiring low computing power for performing the analysis. It can also be a powerful tool to identify the most appropriate physically meaningful theoretical decay function, which best describes the systems under study.