Over the decades efforts have been made to realize the promising potentials of fluorescent quantum dots (QDs) in numerous applications. For that purpose, a mechanistic understanding of fluorescence fluctuations over time in QDs is necessary for synthesizing QDs with desired photophysical properties. While single-particle fluorescence spectroscopy offers an indispensable approach to study the temporal characteristics, the emission behavior of QDs at the single-particle level is complicated in various aspects. With the aim of decoupling the complicating factors, we applied statistical analysis methods to preselect experimental raw data. Following that, we were able to perform quantitative, rigorous studies and discover (1) how fast fluctuations of photoluminescence lifetime exist in compact CdSe/CdS core/shell QDs while the intensity is largely unaffected; and (2) how recombination processes of single QDs near plasmonic gold nanostructures can be modulated by varying the excitation wavelength.

Probing temporal changes in the fluorescence of single quantum dots

ACS Spring 2022

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