Sub-Bandgap Optical Modulation of Quantum Dot Blinking
Statistics
Posted on 2020-07-27 - 17:17
Colloidal
quantum dots (QDs) suffer from pervasive photoluminescence
intermittency that frustrates applications and correlates with irreversible
photodegradation. In single-QD spectroscopies, blinking manifests
as sporadic switching between ON and OFF states without a characteristic
time scale, and the longstanding search for mechanisms has been recently
accelerated by techniques to controllably modulate the QD environment.
Here, we develop an all-optical modulation scheme and demonstrate
that sub-bandgap light tuned to the stimulated emission transition
perturbs the blinking statistics of individual CdSe/ZnS core/shell
QDs. Resonant optical modulation progressively suppresses long-duration
ON events, quantified by a power-law slope that is more negative on
average (ΔαON = 0.46 ±
0.09), while OFF distributions and truncation times are unaffected.
This characteristic effect is robust to choices in background subtraction
and statistical analysis but supports mechanistic descriptions beyond
first-order kinetics. This demonstration of all-optical perturbation
of QD blinking dynamics provides an experimental avenue to disentangle
the complex photophysics of photoluminescence intermittency.
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Hasham, Minhal; Wilson, Mark W. B. (2020). Sub-Bandgap Optical Modulation of Quantum Dot Blinking
Statistics. ACS Publications. Collection. https://doi.org/10.1021/acs.jpclett.0c01599