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Title: Using shape to turn off blinking for two-colour multiexciton emission in CdSe/CdS tetrapods

Here, semiconductor nanostructures capable of emitting from two excited states and thereby of producing two photoluminescence colours are of fundamental and potential technological significance. In this limited class of nanocrystals, CdSe/CdS core/arm tetrapods exhibit the unusual trait of two-colour (red and green) multiexcitonic emission, with green emission from the CdS arms emerging only at high excitation fluences. Here we show that by synthetic shape-tuning, both this multi-colour emission process, and blinking and photobleaching behaviours of single tetrapods can be controlled. Specifically, we find that the properties of dual emission and single-nanostructure photostability depend on different structural parameters—arm length and arm diameter, respectively—but that both properties can be realized in the same nanostructure. Furthermore, based on results of correlated photoluminescence and transient absorption measurements, we conclude that hole-trap filling in the arms and partial state-filling in the core are necessary preconditions for the observation of multiexciton multi-colour emission.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); The Univ. of Texas at Dallas, Richardson, TX (United States)
  3. The Univ. of Texas at Dallas, Richardson, TX (United States)
Publication Date:
Report Number(s):
LA-UR-17-21822
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
Work was performed at CINT, with aspects of the work by CINT User Projects (U2013A0134, U2013B0037); USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Inorganic and Physical Chemistry; Material Science
OSTI Identifier:
1358172

Mishra, Nimai, Orfield, Noah Jeremiah, Wang, Feng, Hu, Zhongjian, Krishnamurthy, Sachidananda, Malko, Anton V., Casson, Joanna Lee, Htoon, Han, Sykora, Milan, and Hollingsworth, Jennifer Ann. Using shape to turn off blinking for two-colour multiexciton emission in CdSe/CdS tetrapods. United States: N. p., Web. doi:10.1038/ncomms15083.
Mishra, Nimai, Orfield, Noah Jeremiah, Wang, Feng, Hu, Zhongjian, Krishnamurthy, Sachidananda, Malko, Anton V., Casson, Joanna Lee, Htoon, Han, Sykora, Milan, & Hollingsworth, Jennifer Ann. Using shape to turn off blinking for two-colour multiexciton emission in CdSe/CdS tetrapods. United States. doi:10.1038/ncomms15083.
Mishra, Nimai, Orfield, Noah Jeremiah, Wang, Feng, Hu, Zhongjian, Krishnamurthy, Sachidananda, Malko, Anton V., Casson, Joanna Lee, Htoon, Han, Sykora, Milan, and Hollingsworth, Jennifer Ann. 2017. "Using shape to turn off blinking for two-colour multiexciton emission in CdSe/CdS tetrapods". United States. doi:10.1038/ncomms15083. https://www.osti.gov/servlets/purl/1358172.
@article{osti_1358172,
title = {Using shape to turn off blinking for two-colour multiexciton emission in CdSe/CdS tetrapods},
author = {Mishra, Nimai and Orfield, Noah Jeremiah and Wang, Feng and Hu, Zhongjian and Krishnamurthy, Sachidananda and Malko, Anton V. and Casson, Joanna Lee and Htoon, Han and Sykora, Milan and Hollingsworth, Jennifer Ann},
abstractNote = {Here, semiconductor nanostructures capable of emitting from two excited states and thereby of producing two photoluminescence colours are of fundamental and potential technological significance. In this limited class of nanocrystals, CdSe/CdS core/arm tetrapods exhibit the unusual trait of two-colour (red and green) multiexcitonic emission, with green emission from the CdS arms emerging only at high excitation fluences. Here we show that by synthetic shape-tuning, both this multi-colour emission process, and blinking and photobleaching behaviours of single tetrapods can be controlled. Specifically, we find that the properties of dual emission and single-nanostructure photostability depend on different structural parameters—arm length and arm diameter, respectively—but that both properties can be realized in the same nanostructure. Furthermore, based on results of correlated photoluminescence and transient absorption measurements, we conclude that hole-trap filling in the arms and partial state-filling in the core are necessary preconditions for the observation of multiexciton multi-colour emission.},
doi = {10.1038/ncomms15083},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {5}
}

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