skip to main content

DOE PAGESDOE PAGES

Title: 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 “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.
Authors:
 [1] ;  [1] ; ORCiD logo [1]
  1. Univ. of Akron, OH (United States). Dept. of Polymer Science
Publication Date:
Grant/Contract Number:
SC0001089; DMR-1665284; CHE-1607138
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
Univ. of Akron, OH (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; coarse-grained models; self-assembly
OSTI Identifier:
1499997

Liu, Zhuonan, Liu, Tianbo, and Tsige, Mesfin. Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation. United States: N. p., 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. 2018. "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}
}

Works referenced in this record:

Self-assembly of ten molecules into nanometre-sized organic host frameworks
journal, November 1995
  • Fujita, Makoto; Oguro, Daichi; Miyazawa, Mayumi
  • Nature, Vol. 378, Issue 6556, p. 469-471
  • DOI: 10.1038/378469a0