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Title: Radiative lifetimes of zincblende CdSe/CdS quantum dots

Abstract

Recent synthetic advances have made available very monodisperse zincblende CdSe/CdS quantum dots having near-unity photoluminescence quantum yields. Because of the absence of nonradiative decay pathways, accurate values of the radiative lifetimes can be obtained from time-resolved PL measurements. Radiative lifetimes can also be obtained from the Einstein relations, using the static absorption spectra and the relative thermal populations in the angular momentum sublevels. We found that one of the inputs into these calculations is the shell thickness, and it is useful to be able to determine shell thickness from spectroscopic measurements. We use an empirically corrected effective mass model to produce a “map” of exciton wavelength as a function of core size and shell thickness. These calculations use an elastic continuum model and the known lattice and elastic constants to include the effect of lattice strain on the band gap energy. The map is in agreement with the known CdSe sizing curve and with the shell thicknesses of zincblende core/shell particles obtained from TEM images. Furthermore, if selenium–sulfur diffusion is included and lattice strain is omitted from the calculation then the resulting map is appropriate for wurtzite CdSe/CdS quantum dots synthesized at high temperatures, and this map is very similarmore » to one previously reported (J. Am. Chem. Soc. 2009, 131, 14299). Radiative lifetimes determined from time-resolved measurements are compared to values obtained from the Einstein relations, and found to be in excellent agreement. For a specific core size (2.64 nm diameter, in the present case), radiative lifetimes are found to decrease with increasing shell thickness. Thus, this is similar to the size dependence of one-component CdSe quantum dots and in contrast to the size dependence in type-II quantum dots.« less

Authors:
 [1];  [2];  [2];  [2];  [1]
  1. Univ. of California, Merced, CA (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). EFRC for Solid State Lighting Science (SSLS); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1235255
Report Number(s):
SAND-2015-20736J
Journal ID: ISSN 1932-7447; 558183
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 119; Journal Issue: 04; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Gong, Ke, Martin, James E., Shea-Rohwer, Lauren E., Lu, Ping, and Kelley, David F. Radiative lifetimes of zincblende CdSe/CdS quantum dots. United States: N. p., 2015. Web. doi:10.1021/jp5118932.
Gong, Ke, Martin, James E., Shea-Rohwer, Lauren E., Lu, Ping, & Kelley, David F. Radiative lifetimes of zincblende CdSe/CdS quantum dots. United States. doi:10.1021/jp5118932.
Gong, Ke, Martin, James E., Shea-Rohwer, Lauren E., Lu, Ping, and Kelley, David F. Fri . "Radiative lifetimes of zincblende CdSe/CdS quantum dots". United States. doi:10.1021/jp5118932. https://www.osti.gov/servlets/purl/1235255.
@article{osti_1235255,
title = {Radiative lifetimes of zincblende CdSe/CdS quantum dots},
author = {Gong, Ke and Martin, James E. and Shea-Rohwer, Lauren E. and Lu, Ping and Kelley, David F.},
abstractNote = {Recent synthetic advances have made available very monodisperse zincblende CdSe/CdS quantum dots having near-unity photoluminescence quantum yields. Because of the absence of nonradiative decay pathways, accurate values of the radiative lifetimes can be obtained from time-resolved PL measurements. Radiative lifetimes can also be obtained from the Einstein relations, using the static absorption spectra and the relative thermal populations in the angular momentum sublevels. We found that one of the inputs into these calculations is the shell thickness, and it is useful to be able to determine shell thickness from spectroscopic measurements. We use an empirically corrected effective mass model to produce a “map” of exciton wavelength as a function of core size and shell thickness. These calculations use an elastic continuum model and the known lattice and elastic constants to include the effect of lattice strain on the band gap energy. The map is in agreement with the known CdSe sizing curve and with the shell thicknesses of zincblende core/shell particles obtained from TEM images. Furthermore, if selenium–sulfur diffusion is included and lattice strain is omitted from the calculation then the resulting map is appropriate for wurtzite CdSe/CdS quantum dots synthesized at high temperatures, and this map is very similar to one previously reported (J. Am. Chem. Soc. 2009, 131, 14299). Radiative lifetimes determined from time-resolved measurements are compared to values obtained from the Einstein relations, and found to be in excellent agreement. For a specific core size (2.64 nm diameter, in the present case), radiative lifetimes are found to decrease with increasing shell thickness. Thus, this is similar to the size dependence of one-component CdSe quantum dots and in contrast to the size dependence in type-II quantum dots.},
doi = {10.1021/jp5118932},
journal = {Journal of Physical Chemistry. C},
number = 04,
volume = 119,
place = {United States},
year = {2015},
month = {1}
}

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