Two-Step Nucleation and Growth of InP Quantum Dots via Magic-Sized Cluster Intermediates
Abstract
We report on the role of magic-sized clusters (MSCs) as key intermediates in the synthesis of indium phosphide quantum dots (InP QDs) from molecular precursors. These observations suggest that previous efforts to control nucleation and growth by tuning precursor reactivity have been undermined by formation of these kinetically persistent MSCs prior to QD formation. The thermal stability of InP MSCs is influenced by the presence of exogenous bases as well as choice of the anionic ligand set. Addition of a primary amine, a common additive in previous InP QD syntheses, to carboxylate terminated MSCs was found to bypass the formation of MSCs, allowing for homogeneous growth of InP QDs through a continuum of isolable sizes. Substitution of the carboxylate ligand set for a phosphonate ligand set increased the thermal stability of one particular InP MSC to 400°C. The structure and optical properties of the MSCs with both carboxylate and phosphonate ligand sets were studied by UV-Vis absorption spectroscopy, powder XRD analysis, and solution ³¹P{¹H} and ¹H NMR spectroscopy. Finally, the carboxylate terminated MSCs were identified as effective single source precursors (SSPs) for the synthesis of high quality InP QDs. Employing InP MSCs as SSPs for QDs effectively decouples the formationmore »
- Authors:
-
- Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry
- Columbia Univ., New York, NY (United States). Dept. of Applied Physics and Applied Mathematics
- Columbia Univ., New York, NY (United States). Dept. of Applied Physics and Applied Mathematics; Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1182518
- Report Number(s):
- BNL-107509-2015-JA
Journal ID: ISSN 0897-4756; R&D Project: PM032; KC0202010
- Grant/Contract Number:
- SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 27; Journal Issue: 4; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; magic-sized clusters (MSCs), indium phosphide quantum dots (InP QDs)
Citation Formats
Gary, Dylan C., Terban, Maxwell W., Billinge, Simon J. L., and Cossairt, Brandi M. Two-Step Nucleation and Growth of InP Quantum Dots via Magic-Sized Cluster Intermediates. United States: N. p., 2015.
Web. doi:10.1021/acs.chemmater.5b00286.
Gary, Dylan C., Terban, Maxwell W., Billinge, Simon J. L., & Cossairt, Brandi M. Two-Step Nucleation and Growth of InP Quantum Dots via Magic-Sized Cluster Intermediates. United States. https://doi.org/10.1021/acs.chemmater.5b00286
Gary, Dylan C., Terban, Maxwell W., Billinge, Simon J. L., and Cossairt, Brandi M. Fri .
"Two-Step Nucleation and Growth of InP Quantum Dots via Magic-Sized Cluster Intermediates". United States. https://doi.org/10.1021/acs.chemmater.5b00286. https://www.osti.gov/servlets/purl/1182518.
@article{osti_1182518,
title = {Two-Step Nucleation and Growth of InP Quantum Dots via Magic-Sized Cluster Intermediates},
author = {Gary, Dylan C. and Terban, Maxwell W. and Billinge, Simon J. L. and Cossairt, Brandi M.},
abstractNote = {We report on the role of magic-sized clusters (MSCs) as key intermediates in the synthesis of indium phosphide quantum dots (InP QDs) from molecular precursors. These observations suggest that previous efforts to control nucleation and growth by tuning precursor reactivity have been undermined by formation of these kinetically persistent MSCs prior to QD formation. The thermal stability of InP MSCs is influenced by the presence of exogenous bases as well as choice of the anionic ligand set. Addition of a primary amine, a common additive in previous InP QD syntheses, to carboxylate terminated MSCs was found to bypass the formation of MSCs, allowing for homogeneous growth of InP QDs through a continuum of isolable sizes. Substitution of the carboxylate ligand set for a phosphonate ligand set increased the thermal stability of one particular InP MSC to 400°C. The structure and optical properties of the MSCs with both carboxylate and phosphonate ligand sets were studied by UV-Vis absorption spectroscopy, powder XRD analysis, and solution ³¹P{¹H} and ¹H NMR spectroscopy. Finally, the carboxylate terminated MSCs were identified as effective single source precursors (SSPs) for the synthesis of high quality InP QDs. Employing InP MSCs as SSPs for QDs effectively decouples the formation of MSCs from the subsequent second nucleation event and growth of InP QDs. The concentration dependence of this SSP reaction, as well as the shape uniformity of particles observed by TEM suggests that the stepwise growth from MSCs directly to QDs proceeds via a second nucleation event rather than an aggregative growth mechanism.},
doi = {10.1021/acs.chemmater.5b00286},
journal = {Chemistry of Materials},
number = 4,
volume = 27,
place = {United States},
year = {Fri Jan 30 00:00:00 EST 2015},
month = {Fri Jan 30 00:00:00 EST 2015}
}
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