Diffusive dynamics of nanoparticles in ultra-confined media
Abstract
Differential dynamic microscopy (DDM) was used to investigate the diffusive dynamics of nanoparticles of diameter 200 400 nm that were strongly confined in a periodic square array of cylindrical nanoposts. The minimum distance between posts was 1.3 5 times the diameter of the nanoparticles. The image structure functions obtained from the DDM analysis were isotropic and could be fit by a stretched exponential function. The relaxation time scaled diffusively across the range of wave vectors studied, and the corresponding scalar diffusivities decreased monotonically with increased confinement. The decrease in diffusivity could be described by models for hindered diffusion that accounted for steric restrictions and hydrodynamic interactions. The stretching exponent decreased linearly as the nanoparticles were increasingly confined by the posts. Altogether, these results are consistent with a picture in which strongly confined nanoparticles experience a heterogeneous spatial environment arising from hydrodynamics and volume exclusion on time scales comparable to cage escape, leading to multiple relaxation processes and Fickian but non-Gaussian diffusive dynamics.
- Authors:
-
- Univ. of Houston, Houston, TX (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1265727
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Soft Matter
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 38; Journal ID: ISSN 1744-683X
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Jacob, Jack Deodato, Conrad, Jacinta, Krishnamoorti, Ramanan, Retterer, Scott T., and He, Kai. Diffusive dynamics of nanoparticles in ultra-confined media. United States: N. p., 2015.
Web. doi:10.1039/C5SM01437A.
Jacob, Jack Deodato, Conrad, Jacinta, Krishnamoorti, Ramanan, Retterer, Scott T., & He, Kai. Diffusive dynamics of nanoparticles in ultra-confined media. United States. https://doi.org/10.1039/C5SM01437A
Jacob, Jack Deodato, Conrad, Jacinta, Krishnamoorti, Ramanan, Retterer, Scott T., and He, Kai. Mon .
"Diffusive dynamics of nanoparticles in ultra-confined media". United States. https://doi.org/10.1039/C5SM01437A. https://www.osti.gov/servlets/purl/1265727.
@article{osti_1265727,
title = {Diffusive dynamics of nanoparticles in ultra-confined media},
author = {Jacob, Jack Deodato and Conrad, Jacinta and Krishnamoorti, Ramanan and Retterer, Scott T. and He, Kai},
abstractNote = {Differential dynamic microscopy (DDM) was used to investigate the diffusive dynamics of nanoparticles of diameter 200 400 nm that were strongly confined in a periodic square array of cylindrical nanoposts. The minimum distance between posts was 1.3 5 times the diameter of the nanoparticles. The image structure functions obtained from the DDM analysis were isotropic and could be fit by a stretched exponential function. The relaxation time scaled diffusively across the range of wave vectors studied, and the corresponding scalar diffusivities decreased monotonically with increased confinement. The decrease in diffusivity could be described by models for hindered diffusion that accounted for steric restrictions and hydrodynamic interactions. The stretching exponent decreased linearly as the nanoparticles were increasingly confined by the posts. Altogether, these results are consistent with a picture in which strongly confined nanoparticles experience a heterogeneous spatial environment arising from hydrodynamics and volume exclusion on time scales comparable to cage escape, leading to multiple relaxation processes and Fickian but non-Gaussian diffusive dynamics.},
doi = {10.1039/C5SM01437A},
journal = {Soft Matter},
number = 38,
volume = 11,
place = {United States},
year = {Mon Aug 10 00:00:00 EDT 2015},
month = {Mon Aug 10 00:00:00 EDT 2015}
}
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