Atomistic simulation of PDADMAC/PSS oligoelectrolyte multilayers: Overall comparison of tri- And tetra-layer systems(Article)(Open Access)
- aUral Federal University, 51 Lenin av., Ekaterinburg, 620000, Russian Federation
- bInstitute of Ion Beam Physics and Materials Research, Helmholtz-Zentrum Dresden-Rossendorf E.V., Dresden, Germany
- cDepartment of Computer Science, Stanford University, Stanford, CA, United States
- dInstitut für Computerphysik, Universität Stuttgart, Stuttgart, 70569, Germany
- eChemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, IL, United States
- fForschungszentrum Jülich, Helmholtz Institute Erlangen-Nuremberg, Nuremberg, Germany
Abstract
By employing large-scale molecular dynamics simulations of atomistically resolved oligoelectrolytes in aqueous solutions, we study in detail the first four layer-by-layer deposition cycles of an oligoelectrolyte multilayer made of poly(diallyl dimethyl ammonium chloride)/poly(styrene sulfonate sodium salt) (PDADMAC/PSS). The multilayers are grown on a silica substrate in 0.1 M NaCl electrolyte solutions and the swollen structures are then subsequently exposed to varying added salt concentration. We investigated the microscopic properties of the films, analyzing in detail the differences between three- and four-layer systems. Our simulations provide insights into the early stages of growth of a multilayer, which are particularly challenging for experimental observations. We found rather strong complexation of the oligoelectrolytes, with fuzzy layering of the film structure. The main charge compensation mechanism is for all cases intrinsic, whereas extrinsic compensation is relatively enhanced for the layer of the last deposition cycle. In addition, we quantified other fundamental observables of these systems, such as the film thickness, water uptake, and overcharge fractions for each deposition layer. This journal is © The Royal Society of Chemistry.
Indexed keywords
| Engineering controlled terms: | DepositionElectrolytesMolecular dynamicsSilicaSodium chlorideStyrene |
|---|---|
| Engineering uncontrolled terms | Atomistic simulationsDeposition cyclesDeposition layersElectrolyte solutionsLarge-scale molecular dynamicsLayer by layer depositionMicroscopic propertiesPoly(diallyl-dimethyl-ammonium chloride) |
| Engineering main heading: | Multilayers |
Funding details
| Funding sponsor | Funding number | Acronym |
|---|---|---|
| SPP 1369 | ||
| Ministerium für Wissenschaft, Forschung und Kunst Baden-Württemberg | MWK | |
| Bundesministerium für Bildung und Frauen | BMBF | |
| Government Council on Grants, Russian Federation |
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1
105 BwGRiD (http://www.bw-grid.de), a member of the German D-Grid initiative, funded by the Ministry for Education and Research (Bundesministerium fuer Bildung und Forschung) and the Ministry for Science, Research and Arts Baden-Wuerttemberg (Ministerium fuer Wissenschaft, Forschung und Kunst Baden-Wuerttemberg).
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2
This research was partially supported by the Deutsche Forschungs-gemeinschaft (DFG) within the Priority Program SPP 1369. P. A. S. acknowledges support from the Act 211 of the Government of the Russian Federation, contract No. 02.A03.21.0006. Simulations were carried out at BwGRiD,105 computing clusters and the Hermit Cray XE6 supercomputer of the High Performance Computing Center Stuttgart (HLRS).
- ISSN: 1744683X
- CODEN: SMOAB
- Source Type: Journal
- Original language: English
- DOI: 10.1039/c9sm02010a
- PubMed ID: 31720676
- Document Type: Article
- Publisher: Royal Society of Chemistry
Sánchez, P.A.; Ural Federal University, 51 Lenin av., Ekaterinburg, Russian Federation;
© Copyright 2019 Elsevier B.V., All rights reserved.
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