% IMPORTANT: The following is UTF-8 encoded. This means that in the presence
% of non-ASCII characters, it will not work with BibTeX 0.99 or older.
% Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or
% “biber”.
@ARTICLE{Banchio:862614,
author = {Banchio, Adolfo J. and Heinen, Marco and Holmqvist, Peter
and Naegele, Gerhard},
title = {{S}hort- and long-time diffusion and dynamic scaling in
suspensions of charged colloidal particles},
journal = {The journal of chemical physics},
volume = {148},
number = {13},
issn = {1089-7690},
address = {Melville, NY},
publisher = {American Institute of Physics},
reportid = {FZJ-2019-02883},
pages = {134902 -},
year = {2018},
abstract = {We report on a comprehensive theory-simulation-experimental
study of collective and self-diffusion in concentrated
suspensions of charge-stabilized colloidal spheres. In
theory and simulation, the spheres are assumed to interact
directly by a hard-core plus screened Coulomb effective pair
potential. The intermediate scattering function, fc(q, t),
is calculated by elaborate accelerated Stokesian dynamics
(ASD) simulations for Brownian systems where many-particle
hydrodynamic interactions (HIs) are fully accounted for,
using a novel extrapolation scheme to a macroscopically
large system size valid for all correlation times. The study
spans the correlation time range from the colloidal
short-time to the long-time regime. Additionally, Brownian
Dynamics (BD) simulation and mode-coupling theory (MCT)
results of fc(q, t) are generated where HIs are neglected.
Using these results, the influence of HIs on collective and
self-diffusion and the accuracy of the MCT method are
quantified. It is shown that HIs enhance collective and
self-diffusion at intermediate and long times. At short
times self-diffusion, and for wavenumbers outside the
structure factor peak region also collective diffusion, are
slowed down by HIs. MCT significantly overestimates the
slowing influence of dynamic particle caging. The dynamic
scattering functions obtained in the ASD simulations are in
overall good agreement with our dynamic light scattering
(DLS) results for a concentration series of charged silica
spheres in an organic solvent mixture, in the experimental
time window and wavenumber range. From the simulation data
for the time derivative of the width function associated
with fc(q, t), there is indication of long-time exponential
decay of fc(q, t), for wavenumbers around the location of
the static structure factor principal peak. The experimental
scattering functions in the probed time range are consistent
with a time-wavenumber factorization scaling behavior of
fc(q, t) that was first reported by Segrè and Pusey [Phys.
Rev. Lett. 77, 771 (1996)] for suspensions of hard spheres.
Our BD simulation and MCT results predict a significant
violation of exact factorization scaling which, however, is
approximately restored according to the ASD results when HIs
are accounted for, consistent with the experimental findings
for fc(q, t). Our study of collective diffusion is amended
by simulation and theoretical results for the
self-intermediate scattering function, fs(q, t), and its
non-Gaussian parameter α2(t) and for the particle mean
squared displacement W(t) and its time derivative. Since
self-diffusion properties are not assessed in standard DLS
measurements, a method to deduce W(t) approximately from
fc(q, t) is theoretically validated},
cin = {ICS-3},
ddc = {530},
cid = {I:(DE-Juel1)ICS-3-20110106},
pnm = {551 - Functional Macromolecules and Complexes (POF3-551)},
pid = {G:(DE-HGF)POF3-551},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:29626910},
UT = {WOS:000429359200053},
doi = {10.1063/1.5017969},
url = {https://juser.fz-juelich.de/record/862614},
}