Role of Surface Morphology on Exciton Recombination in Single Quantum Dot-in-Rods Revealed by Optical and Atomic Structure Correlation.

The physical structure of colloidal quantum dot (QD) nanostructures strongly influences their optical and electronic behavior. A fundamental understanding of this interplay between structure and function is crucial to fully tailor the performance of QDs and their assemblies. Here, by directly correlating the atomic and chemical structure of single CdSe-CdS quantum dot-in-rods with time-resolved fluorescence measurements on the same structures, we identify morphological irregularities at their surfaces that moderate photoluminescence efficiencies. We find that two nonradiative exciton recombination mechanisms are triggered by these imperfections: charging and trap-assisted nonradiative processes. Furthermore, we show that the proximity of the surface defects to the CdSe core of the core-shell structures influences whether the charging or trap-assisted nonradiative channel dominates exciton recombination. Our results extend to other QD nanostructures and emphasize surface roughness as a crucial parameter when designing colloidal QDs with specific excitonic fates.