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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...

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Autores principales: Romero-Sanchez, Ivany, Pihlajamaa, Ilian, Adžić, Natasa, Castellano, Laura E., Stiakakis, Emmanuel, Likos, Christos N., Laurati, Marco
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
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.
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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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