A Library of Selenourea Precursors to PbSe Nanocrystals with Size Distributions near the Homogeneous Limit
摘要:
We report a tunable library of N,N,N'-trisubstituted selenourea precursors and their reaction with lead oleate at 60-150 degrees 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 mu M) and the size following complete precursor conversion (d = 1.7-6.6 nm) to be controlled. Narrow size distributions (sigma = 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-phonon structure and exciton phonon coupling rather than broadening caused by the size distribution.
Use of sulfur and selenium compounds as precursors to nanostructured materials
申请人:THE TRUSTEES OF COLUMBIA UNIVERSITY IN THE CITY OF NEW YORK
公开号:US10253256B2
公开(公告)日:2019-04-09
The presently disclosed subject matter provides processes for preparing nanocrystals, including processes for preparing core-shell nanocrystals. The presently disclosed subject matter also provides sulfur and selenium compounds as precursors to nanostructured materials. The presently disclosed subject matter also provides nanocrystals having a particular particle size distribution.
Reaction of <i>N</i>,<i>N</i>-Dimethylselenocarbamoyl Chloride with Nucleophiles. Preparation of Diselenocarbamates, Selenothiocarbamates, and Selenoureas
Reactions of N,N-dimethylselenocarbamoyl chloride prepared by using LiAlHSeH with nucleophiles such as lithium alkylselenolate, lithium alkylthiolate, and amines afford the corresponding diselenocarbamates, selenothiocarbamates, and selenoureas. The crystal structure of the Se-phenyl N,N-dimethyldiselenocarbamate was also determined by X-ray diffraction.
A Library of Selenourea Precursors to PbSe Nanocrystals with Size Distributions near the Homogeneous Limit
作者:Michael P. Campos、Mark P. Hendricks、Alexander N. Beecher、Willem Walravens、Robert A. Swain、Gregory T. Cleveland、Zeger Hens、Matthew Y. Sfeir、Jonathan S. Owen
DOI:10.1021/jacs.6b11021
日期:2017.2.15
We report a tunable library of N,N,N'-trisubstituted selenourea precursors and their reaction with lead oleate at 60-150 degrees 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 mu M) and the size following complete precursor conversion (d = 1.7-6.6 nm) to be controlled. Narrow size distributions (sigma = 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-phonon structure and exciton phonon coupling rather than broadening caused by the size distribution.
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