skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Mechanistic Understanding of the Growth Kinetics and Dynamics of Nanoparticle Superlattices by Coupling Interparticle Forces from Real-Time Measurements

Abstract

Superlattice structures formed by nanoparticle (NP) self-assembly have attracted increasing attention due to their potential as a novel class of nanomaterials with enhanced physicochemical properties tailored by the assembly structure. However, many key questions remain regarding the correlation between the dynamics of individual NPs and the emerging superlattice patterns. Here we investigated the self-assembly of gold NPs by employing in situ transmission electron microscopy equipped with direct detection camera capabilities, which enabled us to track the rapid motion of individual nanoparticles in real time. By calculating the contributions of Brownian, van der Waals, hydrodynamic, and steric hindrance forces, we obtained a quantitative evaluation of the competitive interactions that drive the assembly process. Such competition between forces over various separations is critical for the kinetics of cluster growth, as well as the superlattice formation. Brownian motion resulted in random particle motions to form small-sized clusters, whose growth dynamics was characterized as reaction-limited aggregation. Subsequently, at relative short-range particle separation, van der Waals force overrode the Brownian force and dominantly drove the assembly process. In the close proximity, a delicate balance between van der Waals and steric hindrance forces surprisingly led to a unique dynamic nature of the assembled superlattice. Our studymore » provides a fundamental understanding of coupling energetics and dynamics of NPs involved in the assembly process, enabling the control and design of the structure of nanoparticle superlattices.« less

Authors:
 [1];  [1];  [1];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
  2. Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States; School of Science, MOE Key Laboratory for Non-equilibrium Synthesis and Modulation of Condensed Matter, State Key Laboratory for Mechanical Behavior of Materials, Xi’an Jiaotong University, Xi’an 710049, China
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1496970
Report Number(s):
PNNL-SA-136036
Journal ID: ISSN 1936-0851
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 12; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English

Citation Formats

Lee, Jaewon, Nakouzi, Elias, Song, Miao, Wang, Bin, Chun, Jaehun, and Li, Dongsheng. Mechanistic Understanding of the Growth Kinetics and Dynamics of Nanoparticle Superlattices by Coupling Interparticle Forces from Real-Time Measurements. United States: N. p., 2018. Web. doi:10.1021/acsnano.8b07880.
Lee, Jaewon, Nakouzi, Elias, Song, Miao, Wang, Bin, Chun, Jaehun, & Li, Dongsheng. Mechanistic Understanding of the Growth Kinetics and Dynamics of Nanoparticle Superlattices by Coupling Interparticle Forces from Real-Time Measurements. United States. doi:10.1021/acsnano.8b07880.
Lee, Jaewon, Nakouzi, Elias, Song, Miao, Wang, Bin, Chun, Jaehun, and Li, Dongsheng. Tue . "Mechanistic Understanding of the Growth Kinetics and Dynamics of Nanoparticle Superlattices by Coupling Interparticle Forces from Real-Time Measurements". United States. doi:10.1021/acsnano.8b07880.
@article{osti_1496970,
title = {Mechanistic Understanding of the Growth Kinetics and Dynamics of Nanoparticle Superlattices by Coupling Interparticle Forces from Real-Time Measurements},
author = {Lee, Jaewon and Nakouzi, Elias and Song, Miao and Wang, Bin and Chun, Jaehun and Li, Dongsheng},
abstractNote = {Superlattice structures formed by nanoparticle (NP) self-assembly have attracted increasing attention due to their potential as a novel class of nanomaterials with enhanced physicochemical properties tailored by the assembly structure. However, many key questions remain regarding the correlation between the dynamics of individual NPs and the emerging superlattice patterns. Here we investigated the self-assembly of gold NPs by employing in situ transmission electron microscopy equipped with direct detection camera capabilities, which enabled us to track the rapid motion of individual nanoparticles in real time. By calculating the contributions of Brownian, van der Waals, hydrodynamic, and steric hindrance forces, we obtained a quantitative evaluation of the competitive interactions that drive the assembly process. Such competition between forces over various separations is critical for the kinetics of cluster growth, as well as the superlattice formation. Brownian motion resulted in random particle motions to form small-sized clusters, whose growth dynamics was characterized as reaction-limited aggregation. Subsequently, at relative short-range particle separation, van der Waals force overrode the Brownian force and dominantly drove the assembly process. In the close proximity, a delicate balance between van der Waals and steric hindrance forces surprisingly led to a unique dynamic nature of the assembled superlattice. Our study provides a fundamental understanding of coupling energetics and dynamics of NPs involved in the assembly process, enabling the control and design of the structure of nanoparticle superlattices.},
doi = {10.1021/acsnano.8b07880},
journal = {ACS Nano},
issn = {1936-0851},
number = 12,
volume = 12,
place = {United States},
year = {2018},
month = {11}
}