Atomistic hybrid<scp>particle‐field</scp>molecular dynamics combined with<scp>slip‐springs</scp>: Restoring entangled dynamics to simulations of polymer melts

Wu, Zhenghao; Kalogirou, Andreas S.; Milano, Giuseppe; Müller‐Plathe, Florian

doi:10.1002/jcc.26428

Cited by 13 publications

(26 citation statements)

References 99 publications

(239 reference statements)

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“…It should be stressed that, in all other structural aspects, hard-core and soft-core models are identical, with the foreseeable and well-understood exception of the pair-correlation function at short distances [2]. The introduction of slip-springs to a soft-core model (hPF or DPD) influences dramatically the polymer dynamics: it restores successfully the proper reptation motion to the softcore models [5][6][7]. However, slip-springs have next to no effect on the knotting probability (figures 4(a) and 5)(a), including for melts under heavy confinement (figure 6(a)).…”

Section: Discussionmentioning

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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Section: Discussionmentioning

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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“…Becerra et al 40 used atomistic simulations to parameterize a single-chain slip-link model for poly(ethylene oxide). Recently Wu et al 41 applied hybrid particle-field atomistic molecular dynamics simulations to a united atom model of PE; in these simulations, the field treatment of the nonbonded interactions makes them effectively soft. Entangled dynamics was recovered by the introduction of SLSPs.…”

Section: Introductionmentioning

confidence: 99%

Dynamics and Rheology of Polymer Melts via Hierarchical Atomistic, Coarse-Grained, and Slip-Spring Simulations

et al. 2021

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A hierarchical (triple scale) simulation methodology is presented for the prediction of the dynamical and rheological properties of high molecular-weight entangled polymer melts. The methodology consists of atomistic, moderately coarse-grained (mCG), and highly coarse-grained slip-spring (SLSP) simulations. At the mCG level, a few chemically bonded atoms are lumped into one coarse-grained bead. At this level, the chemical identity of the underlying atomistic system and the interchain topological constraints (entanglements) are preserved. The mCG interaction potentials are derived by matching local structural distributions of the mCG model to those of the atomistic model through iterative Boltzmann inversion. For matching mCG and atomistic dynamics, the mCG time is scaled by a time scaling factor, which compensates for the lower monomeric friction coefficient of the mCG model than that of the atomistic one. At the SLSP level, multiple Kuhn segments of a polymer chain are represented by one coarse-grained bead. The very soft nonbonded interactions between beads do not prevent chain crossing and, hence, can not capture entanglements. The topological constraints are represented by slip-springs, restricting the lateral motion of polymer chains. A compensating pair potential is used in the SLSP model to keep the static macromolecular properties unaltered upon the introduction of slip-springs. The static and kinetic parameters of the SLSP model are determined based on the lower-level simulation models. Particularly, matching the orientational autocorrelation of the end-to-end vector, we determine the number of slip-springs and calibrate the timescale of the SLSP model. As a test case, the hierarchical methodology is applied to cis-1,4-polybutadiene (cPB) at 413 K. Dynamical single-chain and linear viscoelastic properties of cPB melts are calculated for a broad range of molecular weights, ranging from unentangled to well-entangled chains. The calculations are compared, and found in good agreement, with experimental data from the literature.

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“…These springs were allowed to migrate along the chains and followed their own dynamics of migration, creation, and destruction, which implied a sophisticated method in between conventional molecular dynamics simulations and single-chain models. Similar slip-spring mechanisms were adopted by different groups − and implemented into other coarse-grained methods suffering from the same shortcomings, such as DPD , and the hybrid particle field method . Recently, the Brownian dynamics, DPD, and hybrid-particle-field slip-spring implementations were utilized for dynamical and hierarchical multiscale models. − …”

Section: Introductionmentioning

confidence: 99%

“…Similar slipspring mechanisms were adopted by different groups 48−50 and implemented into other coarse-grained methods suffering from the same shortcomings, such as DPD 51,52 and the hybrid particle field method. 53 Recently, the Brownian dynamics, DPD, and hybrid-particle-field slip-spring implementations were utilized for dynamical and hierarchical multiscale models. 54−56 Given their popularity in soft-matter simulations, the applications of slip-link and slip-spring methods to networks have been surprisingly sparse.…”

Section: ■ Introductionmentioning

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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Atomistic hybridparticle‐fieldmolecular dynamics combined withslip‐springs: Restoring entangled dynamics to simulations of polymer melts

Cited by 13 publications

References 99 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

Dynamics and Rheology of Polymer Melts via Hierarchical Atomistic, Coarse-Grained, and Slip-Spring Simulations

Simulation of Elastomers by Slip-Spring Dissipative Particle Dynamics

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