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Dynamical properties across different coarse-grained models for ionic liquids

Rudzinski, Joseph F. ; Kloth, Sebastian ; Wörner, Svenja ; Pal, Tamisra ; Kremer, Kurt ; Bereau, Tristan ; Vogel, Michael (2021)
Dynamical properties across different coarse-grained models for ionic liquids.
In: Journal of Physics: Condensed Matter, 33 (22)
doi: 10.1088/1361-648X/abe6e1
Article, Bibliographie

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Abstract

Room-temperature ionic liquids (RTILs) stand out among molecular liquids for their rich physicochemical characteristics, including structural and dynamic heterogeneity. The significance of electrostatic interactions in RTILs results in long characteristic length- and timescales, and has motivated the development of a number of coarse-grained (CG) simulation models. In this study, we aim to better understand the connection between certain CG parameterization strategies and the dynamical properties and transferability of the resulting models. We systematically compare five CG models: a model largely parameterized from experimental thermodynamic observables; a refinement of this model to increase its structural accuracy; and three models that reproduce a given set of structural distribution functions by construction, with varying intramolecular parameterizations and reference temperatures. All five CG models display limited structural transferability over temperature, and also result in various effective dynamical speedup factors, relative to a reference atomistic model. On the other hand, the structure-based CG models tend to result in more consistent cation–anion relative diffusion than the thermodynamic-based models, for a single thermodynamic state point. By linking short- and long-timescale dynamical behaviors, we demonstrate that the varying dynamical properties of the different CG models can be largely collapsed onto a single curve, which provides evidence for a route to constructing dynamically-consistent CG models of RTILs.

Item Type: Article
Erschienen: 2021
Creators: Rudzinski, Joseph F. ; Kloth, Sebastian ; Wörner, Svenja ; Pal, Tamisra ; Kremer, Kurt ; Bereau, Tristan ; Vogel, Michael
Type of entry: Bibliographie
Title: Dynamical properties across different coarse-grained models for ionic liquids
Language: English
Date: 4 May 2021
Publisher: IOP Publishing
Journal or Publication Title: Journal of Physics: Condensed Matter
Volume of the journal: 33
Issue Number: 22
Collation: 15 Seiten
DOI: 10.1088/1361-648X/abe6e1
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Abstract:

Room-temperature ionic liquids (RTILs) stand out among molecular liquids for their rich physicochemical characteristics, including structural and dynamic heterogeneity. The significance of electrostatic interactions in RTILs results in long characteristic length- and timescales, and has motivated the development of a number of coarse-grained (CG) simulation models. In this study, we aim to better understand the connection between certain CG parameterization strategies and the dynamical properties and transferability of the resulting models. We systematically compare five CG models: a model largely parameterized from experimental thermodynamic observables; a refinement of this model to increase its structural accuracy; and three models that reproduce a given set of structural distribution functions by construction, with varying intramolecular parameterizations and reference temperatures. All five CG models display limited structural transferability over temperature, and also result in various effective dynamical speedup factors, relative to a reference atomistic model. On the other hand, the structure-based CG models tend to result in more consistent cation–anion relative diffusion than the thermodynamic-based models, for a single thermodynamic state point. By linking short- and long-timescale dynamical behaviors, we demonstrate that the varying dynamical properties of the different CG models can be largely collapsed onto a single curve, which provides evidence for a route to constructing dynamically-consistent CG models of RTILs.

Uncontrolled Keywords: room-temperature ionic liquids, multiscale modeling, coarse-grained dynamics, structural-dynamical relationships
Additional Information:

Art.No.: 224001; Erstveröffentlichung

Divisions: 05 Department of Physics
05 Department of Physics > Institute for condensed matter physics (2021 merged in Institute for Condensed Matter Physics)
05 Department of Physics > Institute for condensed matter physics (2021 merged in Institute for Condensed Matter Physics) > Molekulare Dynamik in kondensierter Materie
Date Deposited: 06 May 2021 13:05
Last Modified: 05 Mar 2024 11:15
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