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Title: Thermodynamic Equilibrium-Driven Formation of Single-Sized Nanocrystals: Reaction Media Tuning CdSe Magic-Sized versus Regular Quantum Dots

Abstract

A concept for the fundamental science of nanoparticle synthesis, thermodynamic equilibrium-driven formation of colloidal single-sized nanoparticle ensembles, is proposed and demonstrated in this manuscript, which addresses the controlled formation of CdSe magic-sized and regular quantum dots (MSQDs and RQDs). During formation, the former are magic-sized nuclei without further growth in size, while the latter experience nucleation and growth. Both MSQDs and RQDs exhibit bandgap emission, while the former have homogeneous spectra broadening only and the latter both homogeneous and inhomogeneous spectra broadening. The former are single-sized and the latter have size distribution. With continuous and homogeneous nucleation, the thermodynamically driven formation of MSQDs was realized via our one-pot noninjection approach, which features highly synthetic reproducibility and large-scale capability. With the proper tuning of the synthetic parameters, such as the nature of the reaction medium, that affect the thermodynamic equilibria, various CdSe MSQDs and RQDs were synthesized discriminately under otherwise identical synthetic formulation and reaction conditions; the reaction media were noncoordinating 1-octadecene, coordinating trioctylphosphine, and mixtures of the two. The nature of Cd precursors, affected also by the reaction media, plays a major role in the formation of MSQDs versus RQDs. The present investigation on the thermodynamically driven formation of CdSemore » single-sized nanoparticles via tuning of the reaction medium, mainly, brings novel insights into the formation mechanism and into the surface ligands of the resulting colloidal nanocrystals. More importantly, the present study provides novel experimental design and approaches to single-sized nanoparticles desired for various applications.« less

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [3];  [1];  [3];  [1];  [4]
  1. SIMS, NRC of Canada
  2. ORNL
  3. IMS, NRC of Canada
  4. National Research Council of Canada
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1036606
DOE Contract Number:  
DE-AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Journal of Physical Chemistry C
Additional Journal Information:
Journal Volume: 114; Journal Issue: 8; Journal ID: ISSN 1932-7447
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; DESIGN; DISTRIBUTION; MIXTURES; NUCLEATION; NUCLEI; QUANTUM DOTS; SPECTRA; SYNTHESIS; THERMODYNAMICS; TUNING

Citation Formats

Yu, Kui, Hu, Michael Z., Wang, Ruibing, Le Piolet, Mickael, Frotey, Marion, Zaman, Md. Badruz, Wu, Xiaohua, Leek, Donald M., Tao, Ye, Wilkinson, Diana, and Li, Chunsheng. Thermodynamic Equilibrium-Driven Formation of Single-Sized Nanocrystals: Reaction Media Tuning CdSe Magic-Sized versus Regular Quantum Dots. United States: N. p., 2010. Web. doi:10.1021/jp909310a.
Yu, Kui, Hu, Michael Z., Wang, Ruibing, Le Piolet, Mickael, Frotey, Marion, Zaman, Md. Badruz, Wu, Xiaohua, Leek, Donald M., Tao, Ye, Wilkinson, Diana, & Li, Chunsheng. Thermodynamic Equilibrium-Driven Formation of Single-Sized Nanocrystals: Reaction Media Tuning CdSe Magic-Sized versus Regular Quantum Dots. United States. https://doi.org/10.1021/jp909310a
Yu, Kui, Hu, Michael Z., Wang, Ruibing, Le Piolet, Mickael, Frotey, Marion, Zaman, Md. Badruz, Wu, Xiaohua, Leek, Donald M., Tao, Ye, Wilkinson, Diana, and Li, Chunsheng. 2010. "Thermodynamic Equilibrium-Driven Formation of Single-Sized Nanocrystals: Reaction Media Tuning CdSe Magic-Sized versus Regular Quantum Dots". United States. https://doi.org/10.1021/jp909310a.
@article{osti_1036606,
title = {Thermodynamic Equilibrium-Driven Formation of Single-Sized Nanocrystals: Reaction Media Tuning CdSe Magic-Sized versus Regular Quantum Dots},
author = {Yu, Kui and Hu, Michael Z. and Wang, Ruibing and Le Piolet, Mickael and Frotey, Marion and Zaman, Md. Badruz and Wu, Xiaohua and Leek, Donald M. and Tao, Ye and Wilkinson, Diana and Li, Chunsheng},
abstractNote = {A concept for the fundamental science of nanoparticle synthesis, thermodynamic equilibrium-driven formation of colloidal single-sized nanoparticle ensembles, is proposed and demonstrated in this manuscript, which addresses the controlled formation of CdSe magic-sized and regular quantum dots (MSQDs and RQDs). During formation, the former are magic-sized nuclei without further growth in size, while the latter experience nucleation and growth. Both MSQDs and RQDs exhibit bandgap emission, while the former have homogeneous spectra broadening only and the latter both homogeneous and inhomogeneous spectra broadening. The former are single-sized and the latter have size distribution. With continuous and homogeneous nucleation, the thermodynamically driven formation of MSQDs was realized via our one-pot noninjection approach, which features highly synthetic reproducibility and large-scale capability. With the proper tuning of the synthetic parameters, such as the nature of the reaction medium, that affect the thermodynamic equilibria, various CdSe MSQDs and RQDs were synthesized discriminately under otherwise identical synthetic formulation and reaction conditions; the reaction media were noncoordinating 1-octadecene, coordinating trioctylphosphine, and mixtures of the two. The nature of Cd precursors, affected also by the reaction media, plays a major role in the formation of MSQDs versus RQDs. The present investigation on the thermodynamically driven formation of CdSe single-sized nanoparticles via tuning of the reaction medium, mainly, brings novel insights into the formation mechanism and into the surface ligands of the resulting colloidal nanocrystals. More importantly, the present study provides novel experimental design and approaches to single-sized nanoparticles desired for various applications.},
doi = {10.1021/jp909310a},
url = {https://www.osti.gov/biblio/1036606}, journal = {Journal of Physical Chemistry C},
issn = {1932-7447},
number = 8,
volume = 114,
place = {United States},
year = {2010},
month = {1}
}