Geometrical Entanglement and Alignment Regulate Self-Organization in Active Ring Polymer Suspensions

We study the emerging self-organization in active ring suspensions, focusing on how the rings' orientational order and geometric entanglement vary with density and spatial confinement. To quantify entanglement, we introduce the wrapping number, a pairwise measure of ring interpenetration, while orientational order is characterized by the alignment of the normal vectors to the rings' osculating planes. Both wrapping number and alignment distinguish active from passive systems, and their combination aptly identifies the self-organized states that emerge with the onset of activity. Mutual-information analysis reveals a significant correlation between the alignment and wrapping number across all considered active conditions. However, self-organization displays a nonmonotonic dependence on the activity-induced entanglement. Specifically, moderate wrapping stabilizes contacts of neighboring aligned rings, while excessive entanglement disrupts the alignment. We show that this competition arises because an increasing entanglement interferes with the planar conformations required to form aligned stacks. Given the simplicity of this microscopic mechanism, analogous effects may occur more generally in polymer systems, where the degree of entanglement is regulated by out-of-equilibrium effects.

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Publication Details

Journal
Journal of Chemical Theory and Computation
Published
2025-11-26
DOI
https://doi.org/10.1021/acs.jctc.5c01300
Primary Topic
Polymer Surface Interaction Studies
Type
article
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article

Geometrical Entanglement and Alignment Regulate Self-Organization in Active Ring Polymer Suspensions

Demian Levis, Emanuele Locatelli, Chantal Valeriani, Cristian Micheletti et al.
Journal of Chemical Theory and Computation
Polymer Surface Interaction Studies
article

Geometrical Entanglement and Alignment Regulate Self-Organization in Active Ring Polymer Suspensions

Demian Levis, Emanuele Locatelli, Chantal Valeriani, Cristian Micheletti, Juan Pablo Miranda-López
article en

Abstract

We study the emerging self-organization in active ring suspensions, focusing on how the rings' orientational order and geometric entanglement vary with density and spatial confinement. To quantify entanglement, we introduce the wrapping number, a pairwise measure of ring interpenetration, while orientational order is characterized by the alignment of the normal vectors to the rings' osculating planes. Both wrapping number and alignment distinguish active from passive systems, and their combination aptly identifies the self-organized states that emerge with the onset of activity. Mutual-information analysis reveals a significant correlation between the alignment and wrapping number across all considered active conditions. However, self-organization displays a nonmonotonic dependence on the activity-induced entanglement. Specifically, moderate wrapping stabilizes contacts of neighboring aligned rings, while excessive entanglement disrupts the alignment. We show that this competition arises because an increasing entanglement interferes with the planar conformations required to form aligned stacks. Given the simplicity of this microscopic mechanism, analogous effects may occur more generally in polymer systems, where the degree of entanglement is regulated by out-of-equilibrium effects.

Journal of Chemical Theory and ComputationVol. 21(23)
Universidad Complutense de Madrid (ES), Scuola Internazionale Superiore di Studi Avanzati (IT), University of Padua (IT), Institute for Cross-Disciplinary Physics and Complex Systems (ES), Istituto Nazionale di Fisica Nucleare, Sezione di Padova (IT), Istituto Nazionale per la Fisica della Materia (IT), Universitat de Barcelona (ES)
Openalex Percentile: Top 66%
Polymer Surface Interaction Studies
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