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Title: Near Surface Nucleation and Particle Mediated Growth of Colloidal Au Nanocrystals

Abstract

During non-classical growth of nanostructures via assembly of primary nuclei, nucleation and assembly are assumed to be distinct processes: nanoparticles nucleate randomly and aggregate to form extended structures through Brownian motion in the presence of long-range attractive interactions. Here we investigate the relationship between these two processes by using in situ AFM, in situ, ex situ and cryo TEM and UV-Vis spectroscopy to observe growth of colloidal gold and simulations to develop a mechanistic model of the process. Our results reveal an inexorable link between nucleation and assembly with nuclei forming almost exclusively within a ~ 1 nm interfacial region of existing particles. The new particles immediately close the gap either through a diffusive jump or via growth of a neck between the seed and new particle, generating aggregates exhibiting features commonly attributed to oriented attachment of independently nucleated particles. The results demonstrate that creation of initial particle interfaces leads to local environments that redirect growth towards non-classical processes.

Authors:
 [1]; ORCiD logo [2];  [3]; ORCiD logo [2];  [4];  [2];  [2]; ORCiD logo [2];  [2]
  1. WASHINGTON STATE UNIV
  2. BATTELLE (PACIFIC NW LAB)
  3. UNIVERSITY PROGRAMS
  4. UNIVERSITY OF WASHINGTON
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1591787
Report Number(s):
PNNL-SA-135333
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 10; Journal Issue: 25
Country of Publication:
United States
Language:
English

Citation Formats

Cheng, Yingwen, Tao, Jinhui, Zhu, Guomin, Soltis, Jennifer A., Legg, Benjamin A., Nakouzi, Elias, De Yoreo, James J., Sushko, Maria L., and Liu, Jun. Near Surface Nucleation and Particle Mediated Growth of Colloidal Au Nanocrystals. United States: N. p., 2018. Web. doi:10.1039/c8nr03408g.
Cheng, Yingwen, Tao, Jinhui, Zhu, Guomin, Soltis, Jennifer A., Legg, Benjamin A., Nakouzi, Elias, De Yoreo, James J., Sushko, Maria L., & Liu, Jun. Near Surface Nucleation and Particle Mediated Growth of Colloidal Au Nanocrystals. United States. doi:10.1039/c8nr03408g.
Cheng, Yingwen, Tao, Jinhui, Zhu, Guomin, Soltis, Jennifer A., Legg, Benjamin A., Nakouzi, Elias, De Yoreo, James J., Sushko, Maria L., and Liu, Jun. Sat . "Near Surface Nucleation and Particle Mediated Growth of Colloidal Au Nanocrystals". United States. doi:10.1039/c8nr03408g.
@article{osti_1591787,
title = {Near Surface Nucleation and Particle Mediated Growth of Colloidal Au Nanocrystals},
author = {Cheng, Yingwen and Tao, Jinhui and Zhu, Guomin and Soltis, Jennifer A. and Legg, Benjamin A. and Nakouzi, Elias and De Yoreo, James J. and Sushko, Maria L. and Liu, Jun},
abstractNote = {During non-classical growth of nanostructures via assembly of primary nuclei, nucleation and assembly are assumed to be distinct processes: nanoparticles nucleate randomly and aggregate to form extended structures through Brownian motion in the presence of long-range attractive interactions. Here we investigate the relationship between these two processes by using in situ AFM, in situ, ex situ and cryo TEM and UV-Vis spectroscopy to observe growth of colloidal gold and simulations to develop a mechanistic model of the process. Our results reveal an inexorable link between nucleation and assembly with nuclei forming almost exclusively within a ~ 1 nm interfacial region of existing particles. The new particles immediately close the gap either through a diffusive jump or via growth of a neck between the seed and new particle, generating aggregates exhibiting features commonly attributed to oriented attachment of independently nucleated particles. The results demonstrate that creation of initial particle interfaces leads to local environments that redirect growth towards non-classical processes.},
doi = {10.1039/c8nr03408g},
journal = {Nanoscale},
number = 25,
volume = 10,
place = {United States},
year = {2018},
month = {7}
}

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