Kremer–Grest Models for Commodity Polymer Melts: Linking Theory, Experiment, and Simulation at the Kuhn Scale

Everaers, Ralf; Karimi–Varzaneh, Hossein Ali; Fleck, Frank; Hojdis, Nils; Svaneborg, Carsten

doi:10.1021/acs.macromol.9b02428

Cited by 138 publications

(213 citation statements)

References 151 publications

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“…The fully flexible chain consists of purely repulsive Lennard-Jones beads and a harmonic bond known to reproduce the same chain structures as finitely extensible (FENE) bonds. This, along with a reported characteristic ratio of C ∞ = 2.1, makes it very similar to the standard Kremer-Grest (KG) model (C ∞,KG = 1.7) [41,42]. We thus refer to it as a KG-like chain.…”

Section: Comparison With Different Modelsmentioning

confidence: 53%

Knotting behaviour of polymer chains in the melt state for soft-core models with and without slip-springs

Alberti

Schneider

et al. 2021

J. Phys.: Condens. Matter

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We analyse the knotting behaviour of linear polymer melts in two types of soft-core models, namely dissipative-particle dynamics and hybrid-particle-field models, as well as their variants with slip-springs which are added to recover entangled polymer dynamics. The probability to form knots is found drastically higher in the hybrid-particle-field model compared to its parent hard-core molecular dynamics model. By comparing the knottedness in dissipative-particle dynamics and hybrid-particle-field models with and without slip-springs, we find the impact of slip-springs on the knotting properties to be negligible. As a dynamic property, we measure the characteristic time of knot formation and destruction, and find it to be (i) of the same order as single-monomer motion and (ii) independent of the chain length in all soft-core models. Knots are therefore formed and destroyed predominantly by the unphysical chain crossing. This work demonstrates that the addition of slip-springs does not alter the knotting behaviour, and it provides a general understanding of knotted structures in these two soft-core models of polymer melts.

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Section: Comparison With Different Modelsmentioning

confidence: 53%

Knotting behaviour of polymer chains in the melt state for soft-core models with and without slip-springs

Alberti

Schneider

et al. 2021

J. Phys.: Condens. Matter

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“…Thermodynamic Driving Force for Assembly. To rationalize our experimental observations, we developed a physical (bead-spring) model [86][87][88][89] for the NC-linker mixtures based on our previous theoretical efforts 33,36 and recent studies of gelforming DNA nanostars 90 . We computed theoretical spinodal boundaries (model and theory details in Supporting Information) for the mixture with respect to the NC volume fraction NC and the linker-to-NC ratio Γ (Figure 4a) using first-order thermodynamic perturbation theory (TPT).…”

Section: Ligandmentioning

confidence: 99%

Assembly of Linked Nanocrystal Colloids by Reversible Covalent Bonds

et al. 2020

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The use of dynamically bonding molecules designed to reversibly link solvent-dispersed nanocrystals (NCs) is a promising strategy to form colloidal assemblies with controlled structure and macroscopic properties. In this work, tin-doped indium oxide NCs are functionalized with ligands that form reversible covalent bonds with linking molecules to drive assembly of NC gels. We monitor gelation using small angle X-ray scattering and characterize how changes in the gel structure affect infrared optical properties arising from the localized surface plasmon resonance of the NCs. The assembly is reversible because of the designed linking chemistry, and we disassemble the gels using two strategies: addition of excess NCs to change the ratio of linking molecules to NCs and addition of a capping molecule that displacesthe linking molecules. The assembly behavior is rationalized using a thermodynamic perturbation theory to compute the phase diagram of the NC-linking molecule mixture. Coarse-grained molecular dynamics simulations reveal the competition between loop and bridge linking motifs essential for understanding NC gelation. This combined experimental, computational, and theoretical work provides a platform for controlling and designing the properties of reversible colloidal assemblies that incorporate NC and solvent compositions beyond those compatible with other contemporary (e.g, DNA-based) linking strategies. File list (2) download file view on ChemRxiv Manuscript.pdf (3.07 MiB) download file view on ChemRxiv Supporting Information.pdf (2.48 MiB)

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“…The lack of chemical details in the model is not a problem when looking for scaling laws or universal behaviour and the KG model has helped to clarify many aspects of the structure and dynamics of polymer chains in the immediate vicinity of surfaces 11,[20][21][22]24,25 . Svaneborg and co-authors 26,27 have recently showed that is it possible, by tuning the chain stiffness (i.e. the Kuhn length), to adapt a generic bead-and-spring polymer model to simulate melts of chemically-specific (at and above the Kuhn length) polymers.…”

Section: Introductionmentioning

confidence: 99%

Effects of Graphite and Plasticizers on the Structure of Highly Entangled Polyisoprene Melts

Giunta

Svaneborg

Karimi–Varzaneh

et al. 2019

ACS Appl. Polym. Mater.

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Using a simple and efficient way to optimise a chemically-specific bead-and-spring model for polymer/surface systems, we analyse the structural properties of high molecular weight polyisoprene (PI) in contact with graphite. We find that, in the vicinity of the graphite, the adsorbed PI chains assume a pancake structure, are highly packed and highly entangled. The addition of plasticizers even with moderate surface affinity guarantees an almost complete surface coverage and forces the polymer chains to detach from the surface and to become less entangled. The softening effect of the plasticizers is observed also in bulk when they are added to the system but are not adsorbed on the surface. Finally, we show that the definition of the thickness of the interface is not unambiguous but depends on the observable used to characterized the melt: it is function of the polymer molecular weight if defined looking at the chain conformation but it becomes independent on the polymer chain length if defined looking at the entanglement density.

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Kremer–Grest Models for Commodity Polymer Melts: Linking Theory, Experiment, and Simulation at the Kuhn Scale

Cited by 138 publications

References 151 publications

Knotting behaviour of polymer chains in the melt state for soft-core models with and without slip-springs

Knotting behaviour of polymer chains in the melt state for soft-core models with and without slip-springs

Assembly of Linked Nanocrystal Colloids by Reversible Covalent Bonds

Effects of Graphite and Plasticizers on the Structure of Highly Entangled Polyisoprene Melts

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