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Orfield NJ, McBride JR, Wang F, et al. Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation. ACS Nano. 2016;10(2):1960-8doi: 10.1021/acsnano.5b05876.
Orfield, N. J., McBride, J. R., Wang, F., Buck, M. R., Keene, J. D., Reid, K. R., Htoon, H., Hollingsworth, J. A., & Rosenthal, S. J. (2016). Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation. ACS nano, 10(2), 1960-8. https://doi.org/10.1021/acsnano.5b05876
Orfield, Noah J, et al. "Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation." ACS nano vol. 10,2 (2016): 1960-8. doi: https://doi.org/10.1021/acsnano.5b05876
Orfield NJ, McBride JR, Wang F, Buck MR, Keene JD, Reid KR, Htoon H, Hollingsworth JA, Rosenthal SJ. Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation. ACS Nano. 2016 Feb 23;10(2):1960-8. doi: 10.1021/acsnano.5b05876. Epub 2016 Feb 05. PMID: 26849531.
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ACS Nano. 2016 Feb 23;10(2):1960-8. doi: 10.1021/acsnano.5b05876. Epub 2016 Feb 05.

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

ACS nano

Noah J Orfield, James R McBride, Feng Wang, Matthew R Buck, Joseph D Keene, Kemar R Reid, Han Htoon, Jennifer A Hollingsworth, Sandra J Rosenthal

Affiliations

  1. Department of Chemistry, Vanderbilt University , Nashville, Tennessee 37235, United States.
  2. Vanderbilt Institute for Nanoscale Science and Engineering, Vanderbilt University , Nashville, Tennessee 37235, United States.
  3. Materials Physics & Applications Division: Center for Integrated Nanotechnologies, Los Alamos National Laboratory , Los Alamos, New Mexico 87545, United States.
  4. Department of Interdisciplinary Materials Science, Vanderbilt University , Nashville, Tennessee 37235, United States.
  5. Department of Physics and Astronomy, Vanderbilt University , Nashville, Tennessee 37235, United States.
  6. Department of Pharmacology, Chemical and Biomolecular Engineering, Vanderbilt University , Nashville, Tennessee 37235, United States.
  7. Materials Science and Technology Division, Oak Ridge National Laboratory , Oak Ridge, Tennessee 37831, United States.

PMID: 26849531 DOI: 10.1021/acsnano.5b05876

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. Herein, 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". Therefore, in contrast to conventional QDs, ensemble photoluminescence quantum yield is principally defined by charging processes rather than the existence of dark g-QDs.

Keywords: correlation; heterogeneity; nanocrystal atomic structure; nanocrystal quantum dot; quantum yield

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