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We are grateful to Alexander Klotz for helpful feedback on the manuscript and for sharing in return his manuscript titled "Chirality Effects in Molecular Chainmail" co-authored with Michael Dimitriyev and Caleb Anderson that has been jointly uploaded on arXiv along with the original draft of this study.74 J. L. M. would like to acknowledge the Erasmus+ Programme for Traineeships for financial support. The project that gave rise to these results received the support of a fellowship from the "la Caixa" Foundation (ID 100010434) and from the European Unions Horizon research and innovation programme under Marie Sklodowska-Curie grant agreement no. 847648. The fellowship code is LCF/BQ/PI20/11760019. S. A. acknowledges support from a Ramon y Cajal Fellowship (ref. RYC2022-037744-I), funded by MICIU/AEI/10.13039/501100011033 and FSE+. C. M. acknowledges support by the European Union - NextGenerationEU, in the framework of the PRIN Project "The Physics of Chromosome Folding" (code: 2022R8YXMR, CUP: G53D23000820006) and by PNRR Mission 4, Component 2, Investment 1.4_CN_00000013_CN-HPC: National Centre for HPC, Big Data and Quantum Computing - spoke 7 (CUP: G93C22000600001). The views and opinions expressed are solely those of the authors and do not necessarily reflect those of the European Union, nor can the European Union be held responsible for them.

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Shape and size tunability of sheets of interlocked ring copolymers

Publicado en:Soft Matter. 20 (33): 6595-6607 - 2024-07-30 20(33), DOI: 10.1039/d4sm00694a

Autores: Luengo-Marquez, Juan; Assenza, Salvatore; Micheletti, Cristian

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Mechanically bonded membranes of interlocked ring polymers are a significant generalization of conventional elastic sheets, where connectivity is provided by covalent bonding, and represent a promising class of topological meta-materials. In this context, two open questions regard the large-scale reverberations of the heterogeneous composition of the rings and the inequivalent modes of interlocking neighboring rings. We address these questions with Langevin dynamics simulations of chainmails with honeycomb-lattice connectivity, where the rings are block copolymers with two segments of different rigidity. We considered various combinations of the relative lengths of the two segments and the patterns of the over- and under-passes linking neighboring rings. We find that varying ring composition and linking patterns have independent and complementary effects. While the former sets the overall size of the chainmail, the latter defines the shape, enabling the selection of starkly different conformation types. Notably, one of the considered linking patterns favors saddle-shaped membranes, providing a first example of spontaneous negative Gaussian curvature in mechanically bonded sheets. The results help establish the extent to which mechanically bonded membranes can differ from conventional elastic ones, particularly for the achievable shape and size tunability. Chainmail size is determined by ring rigidity, while the shape is defined by the linking topology. Suitable tuning of the linking modes shows, for the first time in mechanically bonded membranes, the emergence of negative Gaussian curvature.

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