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Title: Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation

Abstract

Physical variations in colloidal nanostructures give rise to heterogeneity in expressed optical behavior. This correlation between nanoscale structure and function demands interrogation of both atomic structure and photophysics at the level of single nanostructures to be fully understood. In this paper, by conducting detailed analyses of fine atomic structure, chemical composition, and time-resolved single-photon photoluminescence data for the same individual nanocrystals, we reveal inhomogeneity in the quantum yields of single nonblinking “giant” CdSe/CdS core/shell quantum dots (g-QDs). We find that each g-QD possesses distinctive single exciton and biexciton quantum yields that result mainly from variations in the degree of charging, rather than from volume or structure inhomogeneity. We further establish that there is a very limited nonemissive “dark” fraction (<2%) among the studied g-QDs and present direct evidence that the g-QD core must lack inorganic passivation for the g-QD to be “dark”. Finally and therefore, in contrast to conventional QDs, ensemble photoluminescence quantum yield is principally defined by charging processes rather than the existence of dark g-QDs.

Authors:
 [1];  [1];  [2];  [2];  [1];  [1];  [2];  [2];  [3]
  1. Vanderbilt Univ., Nashville, TN (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Vanderbilt Univ., Nashville, TN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1409764
Report Number(s):
LA-UR-17-21870
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
AC52-06NA25396; CHE-1213758; EPS-1004083
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 10; Journal Issue: 2; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; correlation; heterogeneity; nanocrystal atomic structure; nanocrystal quantum dot; quantum yield

Citation Formats

Orfield, Noah J., McBride, James R., Wang, Feng, Buck, Matthew R., Keene, Joseph D., Reid, Kemar R., Htoon, Han, Hollingsworth, Jennifer A., and Rosenthal, Sandra J. Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation. United States: N. p., 2016. Web. doi:10.1021/acsnano.5b05876.
Orfield, Noah J., McBride, James R., Wang, Feng, Buck, Matthew R., Keene, Joseph D., Reid, Kemar R., Htoon, Han, Hollingsworth, Jennifer A., & Rosenthal, Sandra J. Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation. United States. doi:10.1021/acsnano.5b05876.
Orfield, Noah J., McBride, James R., Wang, Feng, Buck, Matthew R., Keene, Joseph D., Reid, Kemar R., Htoon, Han, Hollingsworth, Jennifer A., and Rosenthal, Sandra J. Fri . "Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation". United States. doi:10.1021/acsnano.5b05876. https://www.osti.gov/servlets/purl/1409764.
@article{osti_1409764,
title = {Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation},
author = {Orfield, Noah J. and McBride, James R. and Wang, Feng and Buck, Matthew R. and Keene, Joseph D. and Reid, Kemar R. and Htoon, Han and Hollingsworth, Jennifer A. and Rosenthal, Sandra J.},
abstractNote = {Physical variations in colloidal nanostructures give rise to heterogeneity in expressed optical behavior. This correlation between nanoscale structure and function demands interrogation of both atomic structure and photophysics at the level of single nanostructures to be fully understood. In this paper, by conducting detailed analyses of fine atomic structure, chemical composition, and time-resolved single-photon photoluminescence data for the same individual nanocrystals, we reveal inhomogeneity in the quantum yields of single nonblinking “giant” CdSe/CdS core/shell quantum dots (g-QDs). We find that each g-QD possesses distinctive single exciton and biexciton quantum yields that result mainly from variations in the degree of charging, rather than from volume or structure inhomogeneity. We further establish that there is a very limited nonemissive “dark” fraction (<2%) among the studied g-QDs and present direct evidence that the g-QD core must lack inorganic passivation for the g-QD to be “dark”. Finally and therefore, in contrast to conventional QDs, ensemble photoluminescence quantum yield is principally defined by charging processes rather than the existence of dark g-QDs.},
doi = {10.1021/acsnano.5b05876},
journal = {ACS Nano},
number = 2,
volume = 10,
place = {United States},
year = {2016},
month = {2}
}

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