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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