title: A Library of Selenourea Precursors to PbSe Nanocrystals with Size Distributions near the Homogeneous Limit.
abstract: 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.
authors.affiliation: Department of Chemistry, Columbia University , New York, New York 10027, United States.
authors.forename: Michael P
authors.identifier: 0000-0003-1568-2561
authors.initials: MP
authors.lastname: Campos
authors.affiliation: Department of Chemistry, Columbia University , New York, New York 10027, United States.
authors.forename: Mark P
authors.initials: MP
authors.lastname: Hendricks
authors.affiliation: Department of Chemistry, Columbia University , New York, New York 10027, United States.
authors.forename: Alexander N
authors.initials: AN
authors.lastname: Beecher
authors.affiliation: 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.
authors.forename: Willem
authors.initials: W
authors.lastname: Walravens
authors.affiliation: Department of Chemistry, Columbia University , New York, New York 10027, United States.
authors.forename: Robert A
authors.initials: RA
authors.lastname: Swain
authors.affiliation: Department of Chemistry, Columbia University , New York, New York 10027, United States.
authors.forename: Gregory T
authors.initials: GT
authors.lastname: Cleveland
authors.affiliation: Physics and Chemistry of Nanostructures Group (PCN), Ghent University , B-9000 Ghent, Belgium.|Center of Nano and Biophotonics, Ghent University , B-9000 Ghent, Belgium.
authors.forename: Zeger
authors.identifier: 0000-0002-7041-3375
authors.initials: Z
authors.lastname: Hens
authors.affiliation: Center for Functional Nanomaterials, Brookhaven National Laboratory , Upton, New York 11973, United States.
authors.forename: Matthew Y
authors.identifier: 0000-0001-5619-5722
authors.initials: MY
authors.lastname: Sfeir
authors.affiliation: Department of Chemistry, Columbia University , New York, New York 10027, United States.
authors.forename: Jonathan S
authors.identifier: 0000-0001-5502-3267
authors.initials: JS
authors.lastname: Owen
mesh_terms: D007854:Lead / Q000737:chemistry*; D015394:Molecular Structure; D053758:Nanoparticles / Q000737:chemistry*; D016566:Organoselenium Compounds / Q000737:chemistry*; D010316:Particle Size; D018036:Selenium Compounds / Q000737:chemistry*; D013499:Surface Properties; D014508:Urea / Q000031:analogs & derivatives* / Q000737:chemistry
chemical_list: D016566:Organoselenium Compounds; D018036:Selenium Compounds; C081959:selenourea; C088065:lead selenide; D007854:Lead; D014508:Urea