Advanced

In Silico Synthesis of Microgel Particles

Gnan, Nicoletta; Rovigatti, Lorenzo; Bergman, Maxime LU and Zaccarelli, Emanuela (2017) In Macromolecules 50(21). p.8777-8786
Abstract

Microgels are colloidal-scale particles individually made of cross-linked polymer networks that can swell and deswell in response to external stimuli, such as changes to temperature or pH. Despite a large amount of experimental activities on microgels, a proper theoretical description based on individual particle properties is still missing due to the complexity of the particles. To go one step further, here we propose a novel methodology to assemble realistic microgel particles in silico. We exploit the self-assembly of a binary mixture composed of tetravalent (cross-linkers) and bivalent (monomer beads) patchy particles under spherical confinement in order to produce fully bonded networks. The resulting structure is then used to... (More)

Microgels are colloidal-scale particles individually made of cross-linked polymer networks that can swell and deswell in response to external stimuli, such as changes to temperature or pH. Despite a large amount of experimental activities on microgels, a proper theoretical description based on individual particle properties is still missing due to the complexity of the particles. To go one step further, here we propose a novel methodology to assemble realistic microgel particles in silico. We exploit the self-assembly of a binary mixture composed of tetravalent (cross-linkers) and bivalent (monomer beads) patchy particles under spherical confinement in order to produce fully bonded networks. The resulting structure is then used to generate the initial microgel configuration, which is subsequently simulated with a bead-spring model complemented by a temperature-induced hydrophobic attraction. To validate our assembly protocol, we focus on a small microgel test case and show that we can reproduce the experimental swelling curve by appropriately tuning the confining sphere radius, something that would not be possible with less sophisticated assembly methodologies, e.g., in the case of networks generated from an underlying crystal structure. We further investigate the structure (in reciprocal and real space) and the swelling curves of microgels as a function of temperature, finding that our results are well described by the widely used fuzzy sphere model. This is a first step toward a realistic modeling of microgel particles, which will pave the way for a careful assessment of their elastic properties and effective interactions.

(Less)
Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Macromolecules
volume
50
issue
21
pages
10 pages
publisher
The American Chemical Society
external identifiers
  • scopus:85034048296
  • wos:000415911100051
ISSN
0024-9297
DOI
10.1021/acs.macromol.7b01600
language
English
LU publication?
yes
id
48e8cd4a-f575-4942-b428-79556397626d
date added to LUP
2017-12-08 09:01:18
date last changed
2018-01-16 13:27:16
@article{48e8cd4a-f575-4942-b428-79556397626d,
  abstract     = {<p>Microgels are colloidal-scale particles individually made of cross-linked polymer networks that can swell and deswell in response to external stimuli, such as changes to temperature or pH. Despite a large amount of experimental activities on microgels, a proper theoretical description based on individual particle properties is still missing due to the complexity of the particles. To go one step further, here we propose a novel methodology to assemble realistic microgel particles in silico. We exploit the self-assembly of a binary mixture composed of tetravalent (cross-linkers) and bivalent (monomer beads) patchy particles under spherical confinement in order to produce fully bonded networks. The resulting structure is then used to generate the initial microgel configuration, which is subsequently simulated with a bead-spring model complemented by a temperature-induced hydrophobic attraction. To validate our assembly protocol, we focus on a small microgel test case and show that we can reproduce the experimental swelling curve by appropriately tuning the confining sphere radius, something that would not be possible with less sophisticated assembly methodologies, e.g., in the case of networks generated from an underlying crystal structure. We further investigate the structure (in reciprocal and real space) and the swelling curves of microgels as a function of temperature, finding that our results are well described by the widely used fuzzy sphere model. This is a first step toward a realistic modeling of microgel particles, which will pave the way for a careful assessment of their elastic properties and effective interactions.</p>},
  author       = {Gnan, Nicoletta and Rovigatti, Lorenzo and Bergman, Maxime and Zaccarelli, Emanuela},
  issn         = {0024-9297},
  language     = {eng},
  month        = {11},
  number       = {21},
  pages        = {8777--8786},
  publisher    = {The American Chemical Society},
  series       = {Macromolecules},
  title        = {In Silico Synthesis of Microgel Particles},
  url          = {http://dx.doi.org/10.1021/acs.macromol.7b01600},
  volume       = {50},
  year         = {2017},
}