Maximally stiffening composites require maximally coupled rather than maximally entangled polymer species

Michieletto, Davide; Fitzpatrick, Robert; Robertson‐Anderson, Rae M.

doi:10.1039/c9sm01461f

Cited by 7 publications

(4 citation statements)

References 63 publications

(108 reference statements)

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“…Finally, we highlight that our DEA can be applied to any polymeric system, and we envisage interesting outcomes on entangled blends, composites, , or chimeric polymer systems.…”

Section: Discussionmentioning

confidence: 96%

Dynamical Entanglement and Cooperative Dynamics in Entangled Solutions of Ring and Linear Polymers

Michieletto

Sakaue

2020

ACS Macro Lett.

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Understanding how entanglements affect the behavior of polymeric complex fluids is an open challenge in many fields. To elucidate the nature and consequence of entanglements in dense polymer solutions, we propose a novel method: a "dynamical entanglement analysis" (DEA) to extract spatiotemporal entanglement structures from the pairwise displacement correlation of entangled chains. By applying this method to large-scale molecular dynamics simulations of linear and unknotted, nonconcatenated ring polymers, we find a strong and unexpected cooperative dynamics: the footprint of mutual entrainment between entangled chains. We show that DEA is a powerful and sensitive probe that reveals previously unnoticed and architecture-dependent spatiotemporal structures of dynamical entanglement in polymeric solutions. We also propose a mean-field approximation of our analysis that provides previously under-appreciated physical insights into the dynamics of generic entangled polymers. We envisage DEA will be useful to analyze the dynamical evolution of entanglements in generic polymeric systems such as blends and composites.

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“…Finally, we highlight that our DEA can be applied to any polymeric system, and we envisage interesting outcomes on entangled blends, composites, , or chimeric polymer systems.…”

Section: Discussionmentioning

confidence: 96%

Dynamical Entanglement and Cooperative Dynamics in Entangled Solutions of Ring and Linear Polymers

Michieletto

Sakaue

2020

ACS Macro Lett.

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“…Finally, we highlight that our DEA can be applied to any polymeric system and we envisage interesting outcomes on entangled blends [16], composites [47,48] or chimeric [17] polymer systems.…”

mentioning

confidence: 92%

Dynamical Entanglement and Cooperative Dynamics in Entangled Solutions of Ring and Linear Polymers

Michieletto

Sakaue

2020

Preprint

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Understanding how entanglements affect the behaviour of polymeric complex fluids is an open challenge in many fields. To elucidate the nature and consequence of entanglements in dense polymer solutions, we propose a novel method: a "dynamical entanglement analysis" (DEA) to extract spatio-temporal entanglement structures from the pair-wise displacement correlation of entangled chains. By applying this method to large-scale Molecular Dynamics simulations of linear and unknotted, nonconcatenated ring polymers, we find a strong and unexpected cooperative dynamics: the footprint of mutual entrainment between entangled chains. We show that DEA is a powerful and sensitive probe that reveals previously unnoticed, and architecture-dependent, spatio-temporal structures of dynamical entanglement in polymeric solutions. We also propose a mean-field approximation of our analysis which provides previously underappreciated physical insights into the dynamics of generic entangled polymers. We envisage DEA will be useful to analyse the dynamical evolution of entanglements in generic polymeric systems such as blends and composites.

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“…In fact, DNA is at present largely employed in its simplest geometrical form, i.e. that of a linear or nicked circular (torsionally unconstrained) molecule [8][9][10][11][12]. In spite of this, most of the naturally occurring DNA is under torsional and topological constraints, either because circular and non-nicked (as in bacteria) or because of the binding of proteins that restrict the relative rotation of base-pairs in eukaryotes [13][14][15][16].…”

mentioning

confidence: 99%

Topological Tuning of DNA Mobility in Entangled Solutions of Supercoiled Plasmids

Smrek

Garamella

Robertson‐Anderson

et al. 2020

Preprint

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DNA is increasingly employed for bio and nanotechnology thanks to its exquisite versatility and designability. Most of its use is limited to linearised and torsionally relaxed DNA but non-trivial architectures and torsionally constrained – or supercoiled – DNA plasmids are largely neglected; this is partly due to the limited understanding of how supercoiling affects the rheology of entangled DNA. To address this open question we perform large scale Molecular Dynamics (MD) simulations of entangled solutions of DNA plasmids modelled as twistable chains. We discover that, contrarily to what generally assumed in the literature, larger supercoiling increases the average size of plasmids in the entangled regime. At the same time, we discover that this is accompanied by an unexpected increase of diffusivity. We explain our findings as due to a decrease in inter-plasmids threadings and entanglements.

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Maximally stiffening composites require maximally coupled rather than maximally entangled polymer species

Cited by 7 publications

References 63 publications

Dynamical Entanglement and Cooperative Dynamics in Entangled Solutions of Ring and Linear Polymers

Dynamical Entanglement and Cooperative Dynamics in Entangled Solutions of Ring and Linear Polymers

Dynamical Entanglement and Cooperative Dynamics in Entangled Solutions of Ring and Linear Polymers

Topological Tuning of DNA Mobility in Entangled Solutions of Supercoiled Plasmids

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