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Title: A Library of Selenourea Precursors to PbSe Nanocrystals with Size Distributions near the Homogeneous Limit

Here, we report a tunable library of N,N,N'-trisubstituted selenourea precursors and their reaction with lead oleate at 60–150 °C to form carboxylate-terminated PbSe nanocrystals in quantitative yields. Single exponential conversion kinetics can be tailored over 4 orders of magnitude by adjusting the selenourea structure. The wide range of conversion reactivity allows the extent of nucleation ([nanocrystal] = 4.6–56.7 μM) and the size following complete precursor conversion (d = 1.7–6.6 nm) to be controlled. Narrow size distributions (σ = 0.5–2%) are obtained whose spectral line widths are dominated (73–83%) by the intrinsic single particle spectral broadening, as observed using spectral hole burning measurements. Here, the intrinsic broadening decreases with increasing size (fwhm = 320–65 meV, d = 1.6–4.4 nm) that derives from exciton fine structure and exciton–phonon coupling rather than broadening caused by the size distribution.
Authors:
ORCiD logo [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [1] ; ORCiD logo [3] ; ORCiD logo [4] ; ORCiD logo [1]
  1. Columbia Univ., New York, NY (United States)
  2. Ghent Univ., Ghent (Belgium); Columbia Univ., New York, NY (United States)
  3. Ghent Univ., Ghent (Belgium)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
BNL-204649-2018-JAAM
Journal ID: ISSN 0002-7863
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 6; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1437942

Campos, Michael P., Hendricks, Mark P., Beecher, Alexander N., Walravens, Willem, Swain, Robert A., Cleveland, Gregory T., Hens, Zeger, Sfeir, Matthew Y., and Owen, Jonathan S.. A Library of Selenourea Precursors to PbSe Nanocrystals with Size Distributions near the Homogeneous Limit. United States: N. p., Web. doi:10.1021/jacs.6b11021.
Campos, Michael P., Hendricks, Mark P., Beecher, Alexander N., Walravens, Willem, Swain, Robert A., Cleveland, Gregory T., Hens, Zeger, Sfeir, Matthew Y., & Owen, Jonathan S.. A Library of Selenourea Precursors to PbSe Nanocrystals with Size Distributions near the Homogeneous Limit. United States. doi:10.1021/jacs.6b11021.
Campos, Michael P., Hendricks, Mark P., Beecher, Alexander N., Walravens, Willem, Swain, Robert A., Cleveland, Gregory T., Hens, Zeger, Sfeir, Matthew Y., and Owen, Jonathan S.. 2017. "A Library of Selenourea Precursors to PbSe Nanocrystals with Size Distributions near the Homogeneous Limit". United States. doi:10.1021/jacs.6b11021. https://www.osti.gov/servlets/purl/1437942.
@article{osti_1437942,
title = {A Library of Selenourea Precursors to PbSe Nanocrystals with Size Distributions near the Homogeneous Limit},
author = {Campos, Michael P. and Hendricks, Mark P. and Beecher, Alexander N. and Walravens, Willem and Swain, Robert A. and Cleveland, Gregory T. and Hens, Zeger and Sfeir, Matthew Y. and Owen, Jonathan S.},
abstractNote = {Here, we report a tunable library of N,N,N'-trisubstituted selenourea precursors and their reaction with lead oleate at 60–150 °C to form carboxylate-terminated PbSe nanocrystals in quantitative yields. Single exponential conversion kinetics can be tailored over 4 orders of magnitude by adjusting the selenourea structure. The wide range of conversion reactivity allows the extent of nucleation ([nanocrystal] = 4.6–56.7 μM) and the size following complete precursor conversion (d = 1.7–6.6 nm) to be controlled. Narrow size distributions (σ = 0.5–2%) are obtained whose spectral line widths are dominated (73–83%) by the intrinsic single particle spectral broadening, as observed using spectral hole burning measurements. Here, the intrinsic broadening decreases with increasing size (fwhm = 320–65 meV, d = 1.6–4.4 nm) that derives from exciton fine structure and exciton–phonon coupling rather than broadening caused by the size distribution.},
doi = {10.1021/jacs.6b11021},
journal = {Journal of the American Chemical Society},
number = 6,
volume = 139,
place = {United States},
year = {2017},
month = {1}
}