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Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation

Various soluble hydrophilic macroions can self-assemble into hollow, spherical, monolayered supramolecular “blackberry”-type structures, despite their like-charged nature. However, how the 3-D symmetrical macroions prefer to form 2-D monolayers in bulk solution, especially for the highly symmetrical...

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Detalles Bibliográficos
Autores principales: Liu, Zhuonan, Liu, Tianbo, Tsige, Mesfin
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6117333/
https://www.ncbi.nlm.nih.gov/pubmed/30166571
http://dx.doi.org/10.1038/s41598-018-31533-z
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author Liu, Zhuonan
Liu, Tianbo
Tsige, Mesfin
author_facet Liu, Zhuonan
Liu, Tianbo
Tsige, Mesfin
author_sort Liu, Zhuonan
collection PubMed
description Various soluble hydrophilic macroions can self-assemble into hollow, spherical, monolayered supramolecular “blackberry”-type structures, despite their like-charged nature. However, how the 3-D symmetrical macroions prefer to form 2-D monolayers in bulk solution, especially for the highly symmetrical “Keplerate” polyoxometalates and functionalized C(60) macroions has been a mystery. Through molecular dynamics simulations, using a model specifically designed for macroions in solution, the mechanism of this intriguing symmetry-breaking process is found to be related to the apparently asymmetric charge distribution on the surface of macroions in the equatorial belt area (the area which can be effectively involved in the counterion-mediated attraction). As a result, the electric field lines around macroions during the self-assembly process clearly show that the symmetry-breaking happens at the dimer level effectively defining the plane of the self-assembly. These findings are expected to contribute to our fundamental knowledge of complex solution systems that are found in many fields from materials science to biological phenomena.
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spelling pubmed-61173332018-09-05 Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation Liu, Zhuonan Liu, Tianbo Tsige, Mesfin Sci Rep Article Various soluble hydrophilic macroions can self-assemble into hollow, spherical, monolayered supramolecular “blackberry”-type structures, despite their like-charged nature. However, how the 3-D symmetrical macroions prefer to form 2-D monolayers in bulk solution, especially for the highly symmetrical “Keplerate” polyoxometalates and functionalized C(60) macroions has been a mystery. Through molecular dynamics simulations, using a model specifically designed for macroions in solution, the mechanism of this intriguing symmetry-breaking process is found to be related to the apparently asymmetric charge distribution on the surface of macroions in the equatorial belt area (the area which can be effectively involved in the counterion-mediated attraction). As a result, the electric field lines around macroions during the self-assembly process clearly show that the symmetry-breaking happens at the dimer level effectively defining the plane of the self-assembly. These findings are expected to contribute to our fundamental knowledge of complex solution systems that are found in many fields from materials science to biological phenomena. Nature Publishing Group UK 2018-08-30 /pmc/articles/PMC6117333/ /pubmed/30166571 http://dx.doi.org/10.1038/s41598-018-31533-z Text en © The Author(s) 2018 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Liu, Zhuonan
Liu, Tianbo
Tsige, Mesfin
Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation
title Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation
title_full Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation
title_fullStr Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation
title_full_unstemmed Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation
title_short Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation
title_sort unique symmetry-breaking phenomenon during the self-assembly of macroions elucidated by simulation
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6117333/
https://www.ncbi.nlm.nih.gov/pubmed/30166571
http://dx.doi.org/10.1038/s41598-018-31533-z
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