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Title: Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton–Phonon Coupling and the Optimization of Spectral Linewidths

Abstract

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. Furthermore, our findings offer a general pathway for achieving the narrow spectral linewidths required for many applications of nanocrystals.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)
OSTI Identifier:
1371369
Grant/Contract Number:  
SC0001088; FG02-07ER46454; 5-U54-CA151884-05; W911NF-13-D-0001; CHE-1112825
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 16; Journal Issue: 1; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; solar (photovoltaic); solid state lighting; photosynthesis (natural and artificial); charge transport; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing); semiconductor nanocrystals; colloidal quantum dots; photon-correlation Fourier spectroscopy; spectral linewidth; single-molecule spectroscopy; exciton−phonon coupling; nanoparticle synthesis

Citation Formats

Cui, Jian, Beyler, Andrew P., Coropceanu, Igor, Cleary, Liam, Avila, Thomas R., Chen, Yue, Cordero, José M., Heathcote, S. Leigh, Harris, Daniel K., Chen, Ou, Cao, Jianshu, and Bawendi, Moungi G. Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton–Phonon Coupling and the Optimization of Spectral Linewidths. United States: N. p., 2015. Web. doi:10.1021/acs.nanolett.5b03790.
Cui, Jian, Beyler, Andrew P., Coropceanu, Igor, Cleary, Liam, Avila, Thomas R., Chen, Yue, Cordero, José M., Heathcote, S. Leigh, Harris, Daniel K., Chen, Ou, Cao, Jianshu, & Bawendi, Moungi G. Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton–Phonon Coupling and the Optimization of Spectral Linewidths. United States. doi:10.1021/acs.nanolett.5b03790.
Cui, Jian, Beyler, Andrew P., Coropceanu, Igor, Cleary, Liam, Avila, Thomas R., Chen, Yue, Cordero, José M., Heathcote, S. Leigh, Harris, Daniel K., Chen, Ou, Cao, Jianshu, and Bawendi, Moungi G. Fri . "Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton–Phonon Coupling and the Optimization of Spectral Linewidths". United States. doi:10.1021/acs.nanolett.5b03790. https://www.osti.gov/servlets/purl/1371369.
@article{osti_1371369,
title = {Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton–Phonon Coupling and the Optimization of Spectral Linewidths},
author = {Cui, Jian and Beyler, Andrew P. and Coropceanu, Igor and Cleary, Liam and Avila, Thomas R. and Chen, Yue and Cordero, José M. and Heathcote, S. Leigh and Harris, Daniel K. and Chen, Ou and Cao, Jianshu and Bawendi, Moungi G.},
abstractNote = {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. Furthermore, our findings offer a general pathway for achieving the narrow spectral linewidths required for many applications of nanocrystals.},
doi = {10.1021/acs.nanolett.5b03790},
journal = {Nano Letters},
issn = {1530-6984},
number = 1,
volume = 16,
place = {United States},
year = {2015},
month = {12}
}

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