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J Am Chem Soc. 2017 Feb 15;139(6):2296-2305. doi: 10.1021/jacs.6b11021. Epub 2017 Feb 6.

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

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Department of Chemistry, Columbia University , New York, New York 10027, United States.
Physics and Chemistry of Nanostructures Group (PCN), Ghent University , B-9000 Ghent, Belgium.
Center of Nano and Biophotonics, Ghent University , B-9000 Ghent, Belgium.
Center for Functional Nanomaterials, Brookhaven National Laboratory , Upton, New York 11973, United States.


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. 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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