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Molecular Crowding Increases Knots Abundance in Linear Polymers

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SISSA, International School for Advanced Studies, via Bonomea 265, I-34136 Trieste, Italy
*E-mail [email protected] (G.D.).
Cite this: Macromolecules 2015, 48, 17, 6337–6346
Publication Date (Web):August 17, 2015
https://doi.org/10.1021/acs.macromol.5b01323
Copyright © 2015 American Chemical Society
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    Abstract

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    Stochastic simulations are used to study the effects of molecular crowding on the self-entanglement of linear polymers. We consider flexible chains of beads of up to 1000 monomers and examine how their knotting properties vary in the presence spherical crowders that are 4 times smaller than the chains themselves and which occupy 35% of the solution volume. We find that crowding boosts the incidence of physical knots by more than an order of magnitude for all considered chain lengths. Furthermore, most crowding-induced knots are found to be significantly longer than in the free case. We show that the observed properties follow from the screening of excluded volume interactions mediated by the crowders at length scales larger than their size.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.macromol.5b01323.

    • Additional details for the implicit crowders model; radial distribution functions in the zero-density limit and the depletion thickness; crowding-induced chain compactification, extrapolation for Nm → ∞; typical relaxation times for a chain of beads with/without crowders; selection of genuine physical knots; size of knotted and unknotted subchains; absolute incidence of knots: number of sampled configurations and knotted states (PDF)

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