The capability of quantum dots to generate both single and multiexcitons can be harnessed for a wide variety of applications, including those that require high optical gain. Here, we use time-correlated photoluminescence (PL) spectroscopy to demonstrate that the isolation of single CdSeTe/ZnS core-shell, nanocrystal quantum dots (QDs) in Zero Mode Waveguides (ZMWs) leads to a significant modification in PL intensity, blinking dynamics, and biexciton behavior. QDs in aluminum ZMWs (AlZMWs) exhibited a 15-fold increase in biexciton emission, indicating a preferential enhancement of the biexciton radiative decay rate as compared to the single exciton rate. The increase in biexciton behavior was accompanied by a decrease in blinking events due to a shortening in the dark state residence time. These results indicate that plasmon mediated enhanced decay rates of QDs in AlZMWs lead to substantial changes in the photophysical properties of single quantum dots, including an increase in biexciton behavior.
|Number of pages||9|
|Journal||Journal of Physical Chemistry Letters|
|State||Published - Apr 8 2021|
Bibliographical noteFunding Information:
C.I.R. acknowledges support from HFSP (RGY0081/2014) and NIH (DA038817). Zero-mode waveguides were fabricated at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility.
© 2021 American Chemical Society.
ASJC Scopus subject areas
- Materials Science (all)
- Physical and Theoretical Chemistry