Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation
Abstract
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 C60 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.
- Authors:
-
- Univ. of Akron, OH (United States). Dept. of Polymer Science
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA); Univ. of Akron, OH (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1499997
- Grant/Contract Number:
- SC0001089; DMR-1665284; CHE-1607138
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 8; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; coarse-grained models; self-assembly
Citation Formats
Liu, Zhuonan, Liu, Tianbo, and Tsige, Mesfin. Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation. United States: N. p., 2018.
Web. doi:10.1038/s41598-018-31533-z.
Liu, Zhuonan, Liu, Tianbo, & Tsige, Mesfin. Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation. United States. doi:10.1038/s41598-018-31533-z.
Liu, Zhuonan, Liu, Tianbo, and Tsige, Mesfin. Thu .
"Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation". United States. doi:10.1038/s41598-018-31533-z. https://www.osti.gov/servlets/purl/1499997.
@article{osti_1499997,
title = {Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation},
author = {Liu, Zhuonan and Liu, Tianbo and Tsige, Mesfin},
abstractNote = {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 C60 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.},
doi = {10.1038/s41598-018-31533-z},
journal = {Scientific Reports},
number = ,
volume = 8,
place = {United States},
year = {2018},
month = {8}
}
Web of Science
Figures / Tables:

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Figures / Tables found in this record: