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Title: Super-resolution photoluminescence lifetime and intensity mapping of interacting CdSe/CdS quantum dots

Abstract

We report an optical imaging method that simultaneously achieves nanometer-scale spatial resolution and records single-photon arrival times with subnanosecond temporal resolution, allowing for visualization of nanoscale photoluminescence dynamics. The technique combines time-correlated single-photon counting with single-molecule localization microscopy by monitoring the emission centroid location with a 2 × 2 array of optical fibers that are coupled to four single-photon counting detectors. We applied this method to image isolated and clustered CdSe/CdS core/shell quantum dots (QDs). Single QDs were localized with ~5 nm precision using 104 detected photons. We note within clusters, emission centroids separated by ~12 nm were resolved, and spatial mapping of both the emission intensity and lifetime provided evidence of energy transport pathways among the QDs.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Colorado State Univ., Fort Collins, CO (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC); Gary E. Maciel Fellowship Foundation
OSTI Identifier:
1630862
Alternate Identifier(s):
OSTI ID: 1582485
Report Number(s):
LA-UR-19-30441
Journal ID: ISSN 0003-6951; TRN: US2200702
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 116; Journal Issue: 2; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; Quantum dots; Time-correlated single photon counting; Optical imaging; Optical fibers; Microscopy; Photoluminescence; Image processing

Citation Formats

Dunlap, Megan K., Ryan, Duncan P., Goodwin, Peter M., Werner, James H., Majumder, Somak, Hollingsworth, Jennifer A., Gelfand, Martin P., and Van Orden, Alan. Super-resolution photoluminescence lifetime and intensity mapping of interacting CdSe/CdS quantum dots. United States: N. p., 2020. Web. doi:10.1063/1.5132563.
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Dunlap, Megan K., Ryan, Duncan P., Goodwin, Peter M., Werner, James H., Majumder, Somak, Hollingsworth, Jennifer A., Gelfand, Martin P., & Van Orden, Alan. Super-resolution photoluminescence lifetime and intensity mapping of interacting CdSe/CdS quantum dots. United States. https://doi.org/10.1063/1.5132563
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Dunlap, Megan K., Ryan, Duncan P., Goodwin, Peter M., Werner, James H., Majumder, Somak, Hollingsworth, Jennifer A., Gelfand, Martin P., and Van Orden, Alan. Mon . "Super-resolution photoluminescence lifetime and intensity mapping of interacting CdSe/CdS quantum dots". United States. https://doi.org/10.1063/1.5132563. https://www.osti.gov/servlets/purl/1630862.
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@article{osti_1630862,
title = {Super-resolution photoluminescence lifetime and intensity mapping of interacting CdSe/CdS quantum dots},
author = {Dunlap, Megan K. and Ryan, Duncan P. and Goodwin, Peter M. and Werner, James H. and Majumder, Somak and Hollingsworth, Jennifer A. and Gelfand, Martin P. and Van Orden, Alan},
abstractNote = {We report an optical imaging method that simultaneously achieves nanometer-scale spatial resolution and records single-photon arrival times with subnanosecond temporal resolution, allowing for visualization of nanoscale photoluminescence dynamics. The technique combines time-correlated single-photon counting with single-molecule localization microscopy by monitoring the emission centroid location with a 2 × 2 array of optical fibers that are coupled to four single-photon counting detectors. We applied this method to image isolated and clustered CdSe/CdS core/shell quantum dots (QDs). Single QDs were localized with ~5 nm precision using 104 detected photons. We note within clusters, emission centroids separated by ~12 nm were resolved, and spatial mapping of both the emission intensity and lifetime provided evidence of energy transport pathways among the QDs.},
doi = {10.1063/1.5132563},
journal = {Applied Physics Letters},
number = 2,
volume = 116,
place = {United States},
year = {2020},
month = {1}
}
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https://doi.org/10.1063/1.5132563
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