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Title: Mapping Emission from Clusters of CdSe/ZnS Nanoparticles

Abstract

In this paper, we have carried out correlated super-resolution and SEM imaging studies of clusters of CdSe/ZnS nanoparticles containing up to ten particles to explore how the fluorescence behavior of these clusters depends on the number of particles, the specific cluster geometry, the shell thickness, and the technique used to produce the clusters. The total emission yield was less than proportional to the number of particles in the clusters for both thick and thin shells. With super-resolution imaging, the emission center of the cluster could be spatially resolved at distance scales on the order of the cluster size. The intrinsic fluorescence intermittency of the nanoparticles altered the emission distribution across the cluster, which enabled the identification of relative emission intensities of individual particles or small groups of particles within the cluster. Finally, for clusters undergoing interparticle energy transfer, donor/acceptor pairs and regions where energy was funneled could be identified.

Authors:
 [1];  [2];  [2];  [3];  [1]; ORCiD logo [3]
  1. Colorado State Univ., Fort Collins, CO (United States). Dept. of Physics
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Colorado State Univ., Fort Collins, CO (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Colorado State Univ., Fort Collins, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC); USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)
OSTI Identifier:
1440447
Report Number(s):
LA-UR-18-20821
Journal ID: ISSN 1932-7447
Grant/Contract Number:  
AC52-06NA25396; MPS/CHE-1059089
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 7; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ryan, Duncan P., Goodwin, Peter M., Sheehan, Chris J., Whitcomb, Kevin J., Gelfand, Martin P., and Van Orden, Alan. Mapping Emission from Clusters of CdSe/ZnS Nanoparticles. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.7b10924.
Ryan, Duncan P., Goodwin, Peter M., Sheehan, Chris J., Whitcomb, Kevin J., Gelfand, Martin P., & Van Orden, Alan. Mapping Emission from Clusters of CdSe/ZnS Nanoparticles. United States. doi:10.1021/acs.jpcc.7b10924.
Ryan, Duncan P., Goodwin, Peter M., Sheehan, Chris J., Whitcomb, Kevin J., Gelfand, Martin P., and Van Orden, Alan. Wed . "Mapping Emission from Clusters of CdSe/ZnS Nanoparticles". United States. doi:10.1021/acs.jpcc.7b10924. https://www.osti.gov/servlets/purl/1440447.
@article{osti_1440447,
title = {Mapping Emission from Clusters of CdSe/ZnS Nanoparticles},
author = {Ryan, Duncan P. and Goodwin, Peter M. and Sheehan, Chris J. and Whitcomb, Kevin J. and Gelfand, Martin P. and Van Orden, Alan},
abstractNote = {In this paper, we have carried out correlated super-resolution and SEM imaging studies of clusters of CdSe/ZnS nanoparticles containing up to ten particles to explore how the fluorescence behavior of these clusters depends on the number of particles, the specific cluster geometry, the shell thickness, and the technique used to produce the clusters. The total emission yield was less than proportional to the number of particles in the clusters for both thick and thin shells. With super-resolution imaging, the emission center of the cluster could be spatially resolved at distance scales on the order of the cluster size. The intrinsic fluorescence intermittency of the nanoparticles altered the emission distribution across the cluster, which enabled the identification of relative emission intensities of individual particles or small groups of particles within the cluster. Finally, for clusters undergoing interparticle energy transfer, donor/acceptor pairs and regions where energy was funneled could be identified.},
doi = {10.1021/acs.jpcc.7b10924},
journal = {Journal of Physical Chemistry. C},
number = 7,
volume = 122,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Figure 1 Figure 1: Maximum emission intensity as a function of the number of NPs in a cluster (solid lines). Thick-shell clusters (blue) and thin-shell clusters (green) both produce lower emission rates than would be expected if the intensity were directly proportional to the number of absorbers (dashed lines and encompassing shadedmore » region). Furthermore, thin- and thick-shell NPs have comparable emission reduction. The standard deviation of the maximum intensities of each cluster size group is represented by the shaded regions.« less

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