We use Brownian dynamics simulations and advanced topological profiling methods to characterize the out-of-equilibrium evolution of self-entanglement in linear polymers confined into nanochannels and under periodic compression. By introducing suitable observables, we can distinguish two main forms of entanglement that we term geometrical and topological. The latter is measured by the number of (essential) crossings of the physical knot detected after a suitable bridging of the chain termini. The former is instead measured as the average number of times a linear chain appears to cross itself when viewed under all projections and is irrespective of the physical knotted state. The key discovery of our work is that these two forms of entanglement are uncoupled and evolve with distinct dynamics. While geometrical entanglement is typically in phase with the compression-elongation cycles and it is primarily sensitive to its force f, the topological measure is mildly sensitive to cyclic modulation but strongly depends on both compression force f and duration k. The findings could assist the interpretation of experiments using fluorescence molecular tracers to track physical knots in polymers. Furthermore, we identify optimal regions in the experimentally controllable parameter space in which to obtain more/less topological and geometrical entanglement; this may help designing polymers with targeted topology.

Separation of Geometrical and Topological Entanglement in Confined Polymers Driven out of Equilibrium / Michieletto, D.; Orlandini, E.; Turner, M. S.; Micheletti, C.. - In: ACS MACRO LETTERS. - ISSN 2161-1653. - 9:8(2020), pp. 1081-1085. [10.1021/acsmacrolett.0c00366]

Separation of Geometrical and Topological Entanglement in Confined Polymers Driven out of Equilibrium

Micheletti C.
2020

Abstract

We use Brownian dynamics simulations and advanced topological profiling methods to characterize the out-of-equilibrium evolution of self-entanglement in linear polymers confined into nanochannels and under periodic compression. By introducing suitable observables, we can distinguish two main forms of entanglement that we term geometrical and topological. The latter is measured by the number of (essential) crossings of the physical knot detected after a suitable bridging of the chain termini. The former is instead measured as the average number of times a linear chain appears to cross itself when viewed under all projections and is irrespective of the physical knotted state. The key discovery of our work is that these two forms of entanglement are uncoupled and evolve with distinct dynamics. While geometrical entanglement is typically in phase with the compression-elongation cycles and it is primarily sensitive to its force f, the topological measure is mildly sensitive to cyclic modulation but strongly depends on both compression force f and duration k. The findings could assist the interpretation of experiments using fluorescence molecular tracers to track physical knots in polymers. Furthermore, we identify optimal regions in the experimentally controllable parameter space in which to obtain more/less topological and geometrical entanglement; this may help designing polymers with targeted topology.
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1081
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https://pubs.acs.org/doi/10.1021/acsmacrolett.0c00366
https://arxiv.org/abs/2006.11024v1
Michieletto, D.; Orlandini, E.; Turner, M. S.; Micheletti, C.
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.11767/116389
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