Polymer Chain Collapse upon Rapid Solvent Exchange: Slip-Spring Dissipative Particle Dynamics Simulations with an Explicit-Solvent Model

Schneider, Jurek; Panagiotopoulos, Athanassios Z.; Müller‐Plathe, Florian

doi:10.1021/acs.jpcc.7b07135

Cited by 9 publications

(23 citation statements)

References 33 publications

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“…Depending on the underlying mapping, a DPD bead may represent a few atoms, chain segments, or even entire domains of soft-matter systems. This flexibility along with the low computational costs gives access to mesoscopic time and length scales, making DPD a popular method for the simulation of polymer melts, ,, solutions, − and even elastomeric systems. ,,, In this work, we follow the method of Groot and Warren, where the conservative force is purely linear and defined by a repulsion parameter a ij and a cutoff radius r c . Details can be found in the Simulation Details and ref .…”

Section: Methodsmentioning

confidence: 99%

Simulation of Elastomers by Slip-Spring Dissipative Particle Dynamics

et al. 2021

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We study elastomeric networks using dissipative-particle-dynamics simulations. This soft-core method gives access to mesoscopic time and length scales and is potentially capable to study complex systems such as network defects and gels, but the unmodified method underestimates topological interactions and can only model phantom networks. In this work, we study the capability of slip springs to recover topological effects of network strands. We show that slip springs with a restricted mobility restore the topological contributions of trapped entanglements. Uniaxial strain experiments give access to the cross-link and entanglement contribution to the shear modulus of a slip-spring model network. We find these contributions to coincide with those reported for comparable hard-core Kremer–Grest networks (Gula et al. Macromolecules 2020, 53, 6907–6927). For network strands longer than the chains’ entanglement length, the contribution of slip springs to the shear modulus equals the plateau modulus of the un-cross-linked precursor melt. However, a constant number of slip springs overestimates the shear modulus for high cross-link densities. To probe their applicability, we successfully compare our simulations with experimental polyisoprene rubbers: a network obtained by parameter-free cross-linking of a simulated polyisoprene melt reproduces the viscoelastic moduli of experimental rubbers.

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Section: Methodsmentioning

confidence: 99%

Simulation of Elastomers by Slip-Spring Dissipative Particle Dynamics

et al. 2021

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“…DPD particle interactions consist of a stochastic part, a friction part, and a coarse-grained, soft-core conservative potential. Explicit-solvent DPD has been used for various applications on isolated chains and polymer solutions, some of them featuring single-chain collapse ,, or the precipitation of polymer solutions, so-called flash nanoprecipitation. − It is noteworthy that explicit-solvent DPD simulations fully include hydrodynamics due to their momentum-conserving nature, which is expected to be crucial for a realistic model system. , …”

Section: Methodsmentioning

confidence: 99%

“…Investigation of the coil-to-globule transition of homopolymers has been recognized as an important first step in understanding more complex biological processes such as protein folding and the formation of crumpled chromatin structures . More recently, the development of flash nanoprecipitation , has motivated further studies on polymer collapse and precipitation. − …”

Section: Introductionmentioning

confidence: 99%

Different Stages of Polymer-Chain Collapse Following Solvent Quenching–Scaling Relations from Dissipative Particle Dynamics Simulations

et al. 2020

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We study the collapse of a linear bead-spring chain under a sudden quench in solvent conditions using explicit-solvent dissipative particle dynamics. We investigate the collapse stages of our 50 ≤ N ≤ 1000 bead chains by studying local structures identified by an extended clustering algorithm. We find evidence for the three early stages proposed by Halperin and Goldbart [Phys. Rev. E 2000, 61, 565–573]. Their apparent scaling with the chain length is ∝N 0, N 0.82(6), and N 1.04(2). These values are similar to the predicted ones, and deviations likely stem from the approximations made. The scaling of the overall collapse time with the chain length τc ∝ N 0.94(2), the decay of the squared radius of gyration (R g 2(0) – R g 2(t)) ∝ t 1.09(1), and the growth of blobs along the chain ⟨Sn ⟩ ∝ t 1 are all found to be approximately linear.

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“…Descriptors on the monomer scale [radial distribution function (RDF)], the chain scale (radius of gyration) and bulk scale (density) are identical to within the error bars between soft-core models with and without slip-springs, for the case of polymer melts. (For polymers in solution, there is a small, predictable and well-understood contraction of the radius of gyration [11].) In contrast, there is a structural difference at the monomer scale, e.g.…”

Section: Introductionmentioning

confidence: 99%

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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Polymer Chain Collapse upon Rapid Solvent Exchange: Slip-Spring Dissipative Particle Dynamics Simulations with an Explicit-Solvent Model

Cited by 9 publications

References 33 publications

Simulation of Elastomers by Slip-Spring Dissipative Particle Dynamics

Simulation of Elastomers by Slip-Spring Dissipative Particle Dynamics

Different Stages of Polymer-Chain Collapse Following Solvent Quenching–Scaling Relations from Dissipative Particle Dynamics Simulations

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

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