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Blunt-End Driven Re-entrant Ordering in Quasi Two-Dimensional Dispersions of Spherical DNA Brushes
[Image: see text] We investigate the effects of crowding on the conformations and assembly of confined, highly charged, and thick polyelectrolyte brushes in the osmotic regime. Particle tracking experiments on increasingly dense suspensions of colloids coated with ultralong double-stranded DNA (dsDN...
Autores principales: | , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2022
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8867906/ https://www.ncbi.nlm.nih.gov/pubmed/35130432 http://dx.doi.org/10.1021/acsnano.1c07799 |
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author | Romero-Sanchez, Ivany Pihlajamaa, Ilian Adžić, Natasa Castellano, Laura E. Stiakakis, Emmanuel Likos, Christos N. Laurati, Marco |
author_facet | Romero-Sanchez, Ivany Pihlajamaa, Ilian Adžić, Natasa Castellano, Laura E. Stiakakis, Emmanuel Likos, Christos N. Laurati, Marco |
author_sort | Romero-Sanchez, Ivany |
collection | PubMed |
description | [Image: see text] We investigate the effects of crowding on the conformations and assembly of confined, highly charged, and thick polyelectrolyte brushes in the osmotic regime. Particle tracking experiments on increasingly dense suspensions of colloids coated with ultralong double-stranded DNA (dsDNA) fragments reveal nonmonotonic particle shrinking, aggregation, and re-entrant ordering. Theory and simulations show that aggregation and re-entrant ordering arise from the combined effect of shrinking, which is induced by the osmotic pressure exerted by the counterions absorbed in neighbor brushes and of a short-range attractive interaction competing with electrostatic repulsion. An unconventional mechanism gives origin to the short-range attraction: blunt-end interactions between stretched dsDNA fragments of neighboring brushes, which become sufficiently intense for dense and packed brushes. The attraction can be tuned by inducing free-end backfolding through the addition of monovalent salt. Our results show that base stacking is a mode parallel to hybridization to steer colloidal assembly in which attractions can be fine-tuned through salinity and, potentially, grafting density and temperature. |
format | Online Article Text |
id | pubmed-8867906 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-88679062022-02-24 Blunt-End Driven Re-entrant Ordering in Quasi Two-Dimensional Dispersions of Spherical DNA Brushes Romero-Sanchez, Ivany Pihlajamaa, Ilian Adžić, Natasa Castellano, Laura E. Stiakakis, Emmanuel Likos, Christos N. Laurati, Marco ACS Nano [Image: see text] We investigate the effects of crowding on the conformations and assembly of confined, highly charged, and thick polyelectrolyte brushes in the osmotic regime. Particle tracking experiments on increasingly dense suspensions of colloids coated with ultralong double-stranded DNA (dsDNA) fragments reveal nonmonotonic particle shrinking, aggregation, and re-entrant ordering. Theory and simulations show that aggregation and re-entrant ordering arise from the combined effect of shrinking, which is induced by the osmotic pressure exerted by the counterions absorbed in neighbor brushes and of a short-range attractive interaction competing with electrostatic repulsion. An unconventional mechanism gives origin to the short-range attraction: blunt-end interactions between stretched dsDNA fragments of neighboring brushes, which become sufficiently intense for dense and packed brushes. The attraction can be tuned by inducing free-end backfolding through the addition of monovalent salt. Our results show that base stacking is a mode parallel to hybridization to steer colloidal assembly in which attractions can be fine-tuned through salinity and, potentially, grafting density and temperature. American Chemical Society 2022-02-07 2022-02-22 /pmc/articles/PMC8867906/ /pubmed/35130432 http://dx.doi.org/10.1021/acsnano.1c07799 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Romero-Sanchez, Ivany Pihlajamaa, Ilian Adžić, Natasa Castellano, Laura E. Stiakakis, Emmanuel Likos, Christos N. Laurati, Marco Blunt-End Driven Re-entrant Ordering in Quasi Two-Dimensional Dispersions of Spherical DNA Brushes |
title | Blunt-End
Driven Re-entrant Ordering in Quasi Two-Dimensional
Dispersions of Spherical DNA Brushes |
title_full | Blunt-End
Driven Re-entrant Ordering in Quasi Two-Dimensional
Dispersions of Spherical DNA Brushes |
title_fullStr | Blunt-End
Driven Re-entrant Ordering in Quasi Two-Dimensional
Dispersions of Spherical DNA Brushes |
title_full_unstemmed | Blunt-End
Driven Re-entrant Ordering in Quasi Two-Dimensional
Dispersions of Spherical DNA Brushes |
title_short | Blunt-End
Driven Re-entrant Ordering in Quasi Two-Dimensional
Dispersions of Spherical DNA Brushes |
title_sort | blunt-end
driven re-entrant ordering in quasi two-dimensional
dispersions of spherical dna brushes |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8867906/ https://www.ncbi.nlm.nih.gov/pubmed/35130432 http://dx.doi.org/10.1021/acsnano.1c07799 |
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