Proceedings of nanoGe September Meeting 2017 (NFM17)
Publication date: 20th June 2016
Even after 20 years of research, the phenomenon of blinking of individual quantum dots is poorly understood. Studies usually rely on time-binning the experimental data. The results have been used to propose and validate models for the mechanisms of blinking, involving charging of the quantum dot and/or variable non-radiative recombination rates of excitons. Such models involve excited-state processes with characteristic timescales spanning from nanoseconds (exciton recombination) to seconds (blinking). However, time-binning experimental data sets a limit on the maximum achievable time resolution of the order of a few milliseconds, depending on the count rate from a single quantum dot. This complicates model validation and therefore the understanding of blinking.
Here, we use fluorescence correlation (i.e. photon statistics) to study the full time range from nanoseconds to seconds relevant to the emission dynamics of individual CdSe/CdS quantum dots. In particular, we examine *fast* blinking events on sub-millisecond timescales usually hidden by time binning. Even if the intensity trace seems to show binary ON–OFF blinking, the underlying dynamics may be more complex. A typical single quantum dot randomly switches between periods of efficient optical cycling (ON) and periods of Auger recombination (OFF), but also experiences periods of increased charge-carrier trapping. We discuss how to distinguish quenching due to Auger recombination from quenching due to trapping, and study the dynamics of these processes as a function of CdS shell thickness.
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