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A6:Dynamic heterogeneities in coarse-grained and fine-grained models of liquid crystals and ionic liquids

While the connection between the length scales of simulation models with multiple levels of resolution is provided by the mapping scheme, the link between the different time scales is not known a priori. In this project, we address this problem for two systems exhibiting a range of time scales, namely smectic liquid crystals, and structural and dynamical heterogeneities of ionic liquids. We use dynamic rescaling and Markov state modelling (MSMs) to analyse the kinetic properties of coarse grained (CG) models. A newly developed concept of biasing MSMs helps us to identify sources of kinetic discrepancies and will be used to optimize CG force fields with respect to kinetics and transition barriers.

Dynamical properties across different coarse-grained models for ionic liquids
Joseph F Rudzinski, Sebastian Kloth, Svenja Wörner, Tamisra Pal, Kurt Kremer, Tristan Bereau, Michael Vogel
Journal of Physics: Condensed Matter33 (22),224001 (2021);

Coarse-grained model of a nanoscale-segregated ionic liquid for simulations of low-temperature structure and dynamics
Sebastian Kloth, Marvin P Bernhardt, Nico F A van der Vegt, Michael Vogel
Journal of Physics: Condensed Matter33 (20),204002 (2021);

Coarse-grained conformational surface hopping: Methodology and transferability
Joseph F. Rudzinski and Tristan Bereau
Journal of Chemical Physics153,214110 (2020);
URL: https://doi.org/10.1063/5.0031249

Coarse-grained (CG) conformational surface hopping (SH) adapts the concept of multisurface dynamics, initially developed to describe electronic transitions in chemical reactions, to accurately describe classical molecular dynamics at a reduced level. The SH scheme couples distinct conformational basins (states), each described by its own force field (surface), resulting in a significant improvement of the approximation to the many-body potential of mean force [T. Bereau and J. F. Rudzinski, Phys. Rev. Lett. 121, 256002 (2018)]. The present study first describes CG SH in more detail, through both a toy model and a three-bead model of hexane. We further extend the methodology to non-bonded interactions and report its impact on liquid properties. Finally, we investigate the transferability of the surfaces to distinct systems and thermodynamic state points, through a simple tuning of the state probabilities. In particular, applications to variations in temperature and chemical composition show good agreement with reference atomistic calculations, introducing a promising “weak-transferability regime,” where CG force fields can be shared across thermodynamic and chemical neighborhoods.

Direct route to reproducing pair distribution functions with coarse-grained models via transformed atomistic cross correlations
Svenja J. Wörner, Tristan Bereau, Kurt Kremer, Joseph F. Rudzinski
The Journal of Chemical Physics151 (24),244110 (2019);

Automated detection of many-particle solvation states for accurate characterizations of diffusion kinetics
Joseph F. Rudzinski, Marc Radu, Tristan Bereau
The Journal of Chemical Physics150 (2),024102 (2019);

On the relevance of electrostatic interactions for the structural relaxation of ionic liquids: A molecular dynamics simulation study
Tamisra Pal, Michael Vogel
The Journal of Chemical Physics150 (12),124501 (2019);

Accurate Structure-Based Coarse Graining Leads to Consistent Barrier-Crossing Dynamics
Tristan Bereau, Joseph F. Rudzinski
Physical Review Letters121 (25), (2018);

Effects of Silica Surfaces on the Structure and Dynamics of Room-Temperature Ionic Liquids: A Molecular Dynamics Simulation Study
Tamisra Pal, Constantin Beck, Dominik Lessnich, Michael Vogel
The Journal of Physical Chemistry C122 (1),624-634 (2017);

Single molecule translocation in smectics illustrates the challenge for time-mapping in simulations on multiple scales
Biswaroop Mukherjee, Christine Peter, Kurt Kremer
The Journal of Chemical Physics147 (11),114501 (2017);

Role of Dynamic Heterogeneities in Ionic Liquids: Insights from All-Atom and Coarse-Grained Molecular Dynamics Simulation Studies
Tamisra Pal, Michael Vogel
ChemPhysChem18 (16),2233-2242 (2017);

Computational materials discovery in soft matter
T. Bereau, D. Andrienko, K. Kremer
APL Mat4,053101 (2016);

Soft matter embodies a wide range of materials, which all share the common characteristics of weak interaction energies determining their supramolecular structure. This complicates structure-property predictions and hampers the direct application of data-driven approaches to their modeling. We present several aspects in which these methods play a role in designing soft-matter materials: drug design as well as information-driven computer simulations, e.g., histogram reweighting. We also discuss recent examples of rational design of soft-matter materials fostered by physical insight and assisted by data-driven approaches. We foresee the combination of data-driven and physical approaches a promising strategy to move the field forward.

Concurrent parametrization against static and kinetic information leads to more robust coarse-grained force fields
J.F. Rudzinski, T. Bereau
The European Physical Journal Special Topics225 (8-9),1373-1389 (2016);

Communication: Consistent interpretation of molecular simulation kinetics using Markov state models biased with external information
Joseph F. Rudzinski, Kurt Kremer, Tristan Bereau
The Journal of Chemical Physics144 (5),051102 (2016);

A molecular dynamics simulations study on the relations between dynamical heterogeneity, structural relaxation, and self-diffusion in viscous liquids
Patrick Henritzi, André Bormuth, Felix Klameth, Michael Vogel
The Journal of Chemical Physics143 (16),164502 (2015);


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