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Title: Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals

Abstract

Toward a truly photostable PbSe quantum dot (QD), we apply the thick-shell or “giant” QD structural motif to this notoriously environmentally sensitive nanocrystal system. Namely, using a sequential application of two shell-growth techniques—partial-cation exchange and successive ionic layer adsorption and reaction (SILAR)—we are able to overcoat the PbSe QDs with sufficiently thick CdSe shells to impart new single-QD-level photostability, as evidenced by suppression of both photobleaching and blinking behavior. Here, we further reveal that the crystal structure of the CdSe shell (cubic zinc-blende or hexagonal wurtzite) plays a key role in determining the photoluminescence properties of these giant QDs, with only cubic nanocrystals sufficiently bright and stable to be observed as single emitters. Moreover, we demonstrate that crystal structure and particle shape (cubic, spherical, or tetrapodal) and, thereby, emission properties can be synthetically tuned by either withholding or including the coordinating ligand, trioctylphosphine, in the SILAR component of the shell-growth process.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [2];  [1];  [3]; ORCiD logo [4];  [2];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. of Texas at Dallas, Richardson, TX (United States). Dept. of Physics
  3. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemistry
  4. Univ. of Texas at Dallas, Richardson, TX (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1481991
Report Number(s):
LA-UR-18-21088
Journal ID: ISSN 0002-7863
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 32; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; Inorganic and Physical Chemistry; Material Science

Citation Formats

Hanson, Christina J., Hartmann, Nicolai F., Singh, Ajay, Ma, Xuedan, DeBenedetti, William J. I., Casson, Joanna L., Grey, John K., Chabal, Yves J., Malko, Anton V., Sykora, Milan, Piryatinski, Andrei, Htoon, Han, and Hollingsworth, Jennifer A. Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals. United States: N. p., 2017. Web. doi:10.1021/jacs.7b03705.
Hanson, Christina J., Hartmann, Nicolai F., Singh, Ajay, Ma, Xuedan, DeBenedetti, William J. I., Casson, Joanna L., Grey, John K., Chabal, Yves J., Malko, Anton V., Sykora, Milan, Piryatinski, Andrei, Htoon, Han, & Hollingsworth, Jennifer A. Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals. United States. https://doi.org/10.1021/jacs.7b03705
Hanson, Christina J., Hartmann, Nicolai F., Singh, Ajay, Ma, Xuedan, DeBenedetti, William J. I., Casson, Joanna L., Grey, John K., Chabal, Yves J., Malko, Anton V., Sykora, Milan, Piryatinski, Andrei, Htoon, Han, and Hollingsworth, Jennifer A. Thu . "Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals". United States. https://doi.org/10.1021/jacs.7b03705. https://www.osti.gov/servlets/purl/1481991.
@article{osti_1481991,
title = {Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals},
author = {Hanson, Christina J. and Hartmann, Nicolai F. and Singh, Ajay and Ma, Xuedan and DeBenedetti, William J. I. and Casson, Joanna L. and Grey, John K. and Chabal, Yves J. and Malko, Anton V. and Sykora, Milan and Piryatinski, Andrei and Htoon, Han and Hollingsworth, Jennifer A.},
abstractNote = {Toward a truly photostable PbSe quantum dot (QD), we apply the thick-shell or “giant” QD structural motif to this notoriously environmentally sensitive nanocrystal system. Namely, using a sequential application of two shell-growth techniques—partial-cation exchange and successive ionic layer adsorption and reaction (SILAR)—we are able to overcoat the PbSe QDs with sufficiently thick CdSe shells to impart new single-QD-level photostability, as evidenced by suppression of both photobleaching and blinking behavior. Here, we further reveal that the crystal structure of the CdSe shell (cubic zinc-blende or hexagonal wurtzite) plays a key role in determining the photoluminescence properties of these giant QDs, with only cubic nanocrystals sufficiently bright and stable to be observed as single emitters. Moreover, we demonstrate that crystal structure and particle shape (cubic, spherical, or tetrapodal) and, thereby, emission properties can be synthetically tuned by either withholding or including the coordinating ligand, trioctylphosphine, in the SILAR component of the shell-growth process.},
doi = {10.1021/jacs.7b03705},
url = {https://www.osti.gov/biblio/1481991}, journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 32,
volume = 139,
place = {United States},
year = {2017},
month = {8}
}

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Works referencing / citing this record:

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