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

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.

doi:10.1021/jacs.6b11021

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

Journal Article · Thu Jan 19 00:00:00 EST 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.6b11021· OSTI ID:1437942

^[1]; Hendricks, Mark P. ^[1]; Beecher, Alexander N. ^[1]; Walravens, Willem ^[2]; Swain, Robert A. ^[1]; Cleveland, Gregory T. ^[1];

^[3];

^[4];

^[1]

Columbia Univ., New York, NY (United States)
Ghent Univ., Ghent (Belgium); Columbia Univ., New York, NY (United States)
Ghent Univ., Ghent (Belgium)
Brookhaven National Lab. (BNL), Upton, NY (United States)

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1437942

Report Number(s):: BNL-204649-2018-JAAM

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 6; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 84 works

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CCDC 1577886: Experimental Crystal Structure Determination: ADIWES : N'-cyclohexyl-N,N-diethylselenourea Campos, Michael P.; Hendricks, Mark P.; Beecher, Alexander N. https://doi.org/10.5517/ccdc.csd.cc1pyxk3 The current record is supplemented by this dataset	dataset	October 2017
CCDC 1577883: Experimental Crystal Structure Determination: ADIVOB : N'-cyclohexyl-N-methyl-N-propan-2-ylselenourea Campos, Michael; Hendricks, Mark; Beecher, Alexander https://doi.org/10.5517/ccdc.csd.cc1pyxg0 The current record is supplemented by this dataset	dataset	October 2017
CCDC 1577895: Experimental Crystal Structure Determination: ADIYAQ : N-butylpyrrolidine-1-carboselenoamide Campos, Michael; Hendricks, Mark; Beecher, Alexander https://doi.org/10.5517/ccdc.csd.cc1pyxvd The current record is supplemented by this dataset	dataset	October 2017