Ultraviolet ZnSe1–xSx gradient-alloyed nanocrystals via a noninjection approach

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DOIResolve DOI: http://doi.org/10.1021/am3009828
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TypeArticle
Journal titleACS Applied Materials and Interfaces
ISSN1944-8244
1944-8252
Volume4
Issue8
Pages43024311; # of pages: 10
Subjectalloyed ZnSeS nanocrystals; colloidal quantum dots; photoluminescent; diphenylphosphine; noninjection approach
AbstractHighly emissive ultraviolet ZnSeS nanocrystals (NCs), with a core–shell-like structure, were designed and synthesized via a one-step noninjection approach in 1-octadecene (ODE). These ultraviolet ZnSeS NCs exhibit bright bandgap emission with high color purity and little trap emission. With full width at half-maximum (fwhm) of 21 nm only, photoluminescent (PL) quantum yield (QY) of 60% was estimated for one ensemble dispersed in toluene exhibiting bandgap absorption peaking at 380 nm and bandgap emission at 389 nm. These alloyed ZnSeS NCs present a cubic crystal structure consisting of a Se-rich core and a S-rich shell. Such a gradiently alloyed structure was suggested by our investigation on the temporal evolution of optical properties of the growing ZnSeS NCs monitored from 80 to 300 °C, together with structural and compositional characterization performed with XRD, XPS, EDX, and TEM. This newly developed one-step noninjection approach was achieved with zinc oleate (Zn(OA)2), diphenylphosphine selenide (SeDPP), and diphenylphosphine sulfide (SDPP) as Zn, Se, and S precursors, respectively. ZnSe monomers mainly participated in nucleation at 120 °C, while both ZnSe and ZnS monomers contributed to NC formation in later growth stages (160 °C and higher). 31P NMR study demonstrates that SeDPP is more reactive than SDPP toward Zn(OA)2, and also supports such a model proposed on the combination of ZnSe and ZnS monomers leading to nucleation/growth of ZnSeS alloyed NCs. The present study offers conceptual methodology to various highly photoluminescent alloyed NCs with high quality, high particle yield, and high synthetic reproducibility.
Publication date
LanguageEnglish
AffiliationNational Research Council Canada; NRC Steacie Institute for Molecular Sciences; NRC Institute for Chemical Process and Environmental Technology; NRC Institute for Microstructural Sciences
Peer reviewedYes
NPARC number21269022
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Record identifierb0f73fb5-381d-4b11-ba12-5b63c66ca781
Record created2013-12-02
Record modified2016-05-09
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