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Baig, Chunggi
Theoretical and Computational Study of Polymers & Nanomaterials Lab.
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dc.citation.endPage 124904-16 -
dc.citation.number 12 -
dc.citation.startPage 124904-1 -
dc.citation.title JOURNAL OF CHEMICAL PHYSICS -
dc.citation.volume 132 -
dc.contributor.author Stephanou, Pavlos S. -
dc.contributor.author Baig, Chunggi -
dc.contributor.author Tsolou, Georgia -
dc.contributor.author Mavrantzas, Vlasis G. -
dc.contributor.author Kroeger, Martin -
dc.date.accessioned 2023-12-22T07:12:05Z -
dc.date.available 2023-12-22T07:12:05Z -
dc.date.created 2014-10-07 -
dc.date.issued 2010-03 -
dc.description.abstract The topological state of entangled polymers has been analyzed recently in terms of primitive paths which allowed obtaining reliable predictions of the static (statistical) properties of the underlying entanglement network for a number of polymer melts. Through a systematic methodology that first maps atomistic molecular dynamics (MD) trajectories onto time trajectories of primitive chains and then documents primitive chain motion in terms of a curvilinear diffusion in a tubelike region around the coarse-grained chain contour, we are extending these static approaches here even further by computing the most fundamental function of the reptation theory, namely, the probability ψ (s,t) that a segment s of the primitive chain remains inside the initial tube after time t, accounting directly for contour length fluctuations and constraint release. The effective diameter of the tube is independently evaluated by observing tube constraints either on atomistic displacements or on the displacement of primitive chain segments orthogonal to the initial primitive path. Having computed the tube diameter, the tube itself around each primitive path is constructed by visiting each entanglement strand along the primitive path one after the other and approximating it by the space of a small cylinder having the same axis as the entanglement strand itself and a diameter equal to the estimated effective tube diameter. Reptation of the primitive chain longitudinally inside the effective constraining tube as well as local transverse fluctuations of the chain driven mainly from constraint release and regeneration mechanisms are evident in the simulation results; the latter causes parts of the chains to venture outside their average tube surface for certain periods of time. The computed ψ (s,t) curves account directly for both of these phenomena, as well as for contour length fluctuations, since all of them are automatically captured in the atomistic simulations. Linear viscoelastic properties such as the zero shear rate viscosity and the spectra of storage and loss moduli obtained on the basis of the obtained ψ (s,t) curves for three different polymer melts (polyethylene, cis-1,4-polybutadiene, and trans-1,4-polybutadiene) are consistent with experimental rheological data and in qualitative agreement with the double reptation and dual constraint models. The new methodology is general and can be routinely applied to analyze primitive path dynamics and chain reptation in atomistic trajectories (accumulated through long MD simulations) of other model polymers or polymeric systems (e.g., bidisperse, branched, grafted, etc.); it is thus believed to be particularly useful in the future in evaluating proposed tube models and developing more accurate theories for entangled systems. -
dc.identifier.bibliographicCitation JOURNAL OF CHEMICAL PHYSICS, v.132, no.12, pp.124904-1 - 124904-16 -
dc.identifier.doi 10.1063/1.3361674 -
dc.identifier.issn 0021-9606 -
dc.identifier.scopusid 2-s2.0-77950442774 -
dc.identifier.uri https://scholarworks.unist.ac.kr/handle/201301/6953 -
dc.identifier.url https://aip.scitation.org/doi/10.1063/1.3361674 -
dc.identifier.wosid 000276209700045 -
dc.language 영어 -
dc.publisher AMER INST PHYSICS -
dc.title Quantifying chain reptation in entangled polymer melts: Topological and dynamical mapping of atomistic simulation results onto the tube model -
dc.type Article -
dc.description.isOpenAccess FALSE -
dc.description.journalRegisteredClass scie -
dc.description.journalRegisteredClass scopus -

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