Journal
NANO LETTERS
Volume 16, Issue 1, Pages 289-296Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.5b03790
Keywords
semiconductor nanocrystals; colloidal quantum dots; photon-correlation Fourier spectroscopy; spectral linewidth; single-molecule spectroscopy; exciton-phonon coupling; nanoparticle synthesis
Categories
Funding
- United States Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-FG02-07ER46454]
- National Institutes of Health [5-U54-CA151884-05]
- Army Research Office through the Institute for Soldier Nanotechnologies [W911NF-13-D-0001]
- National Science Foundation [CHE-1112825]
- Center for Excitonics, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0001088]
- National Science Foundation Graduate Research Fellowship Program
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1112825] Funding Source: National Science Foundation
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The optimization of photoluminescence spectral linewidths in semiconductor nanocrystal preparations involves minimizing both the homogeneous and inhomogeneous contributions to the ensemble spectrum. Although the inhomogeneous contribution can be controlled by eliminating interparticle inhomogeneities, far less is known about how to synthetically control the homogeneous, or single-nanocrystal, spectral linewidth. Here, we use,solution photon-correlation Fourier spectroscopy (S-PCFS) to measure how the sample-averaged single-nanocrystal emission linewidth of CdSe core and core/shell nanocrystals change with systematic changes in the size of the cores and the thickness and composition of the shells. We find that the single-nanocrystal linewidth at room temperature is heavily influenced by the nature of the CdSe surface and the epitaxial shell, which have a profound impact on the internal electric fields that affect exciton-phonon coupling. Our results explain the wide variations, both experimental and theoretical, in the magnitude and size dependence in previous reports on exciton-phonon coupling in CdSe nanocrystals. Moreover, our findings offer a general pathway for achieving the narrow spectral linewidths required for many applications of nanocrystals.
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