Like-charge polymer-membrane complexation mediated by multivalent cations: one-loop-dressed strong coupling theory

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buir.contributor.authorBüyükdağlı, Şahin
dc.citation.epage094902-18en_US
dc.citation.issueNumber9en_US
dc.citation.spage094902-1en_US
dc.citation.volumeNumber151en_US
dc.contributor.authorBüyükdağlı, Şahinen_US
dc.contributor.authorPodgornik, R.en_US
dc.date.accessioned2020-02-11T12:58:43Z
dc.date.available2020-02-11T12:58:43Z
dc.date.issued2019
dc.departmentDepartment of Physicsen_US
dc.description.abstractWe probe the electrostatic mechanism driving adsorption of polyelectrolytes onto like-charged membranes upon the addition of tri- and tetravalent counterions to a bathing monovalent salt solution. We develop a one-loop-dressed strong coupling theory that treats the monovalent salt at the electrostatic one-loop level and the multivalent counterions within a strong-coupling approach. It is shown that the adhesive force of the multivalent counterions mediating the like-charge adsorption arises from their strong condensation at the charged membrane. The resulting interfacial counterion excess locally maximizes the screening ability of the electrolyte and minimizes the electrostatic polymer grand potential. This translates into an attractive force that pulls the polymer to the similarly charged membrane. We show that the high counterion valency enables this adsorption transition even at weakly charged membranes. Additionally, strongly charged membranes give rise to monovalent counterion-induced correlations and intensify the interfacial multivalent counterion condensation, strengthening the complexation of the polymer with the like-charged membrane, as well as triggering the orientational transition of the molecule prior to its adsorption. Finally, our theory provides two additional key features as evidenced by previous adsorption experiments: first, the critical counterion concentration for polymer adsorption decreases with the rise of the counterion valency and, second, the addition of monovalent salt enhances the screening of the membrane charges and suppresses monovalent counterion correlations close to the surface. This weakens the interfacial multivalent counterion condensation and results in the desorption of the polymer from the substrate.en_US
dc.identifier.doi10.1063/1.5109637en_US
dc.identifier.issn0021-9606
dc.identifier.urihttp://hdl.handle.net/11693/53286
dc.language.isoEnglishen_US
dc.publisherAmerican Institute of Physicsen_US
dc.relation.isversionofhttps://dx.doi.org/10.1063/1.5109637en_US
dc.source.titleJournal of Chemical Physicsen_US
dc.subjectAdsorptionen_US
dc.subjectPolyelectrolytesen_US
dc.subjectElectrolytesen_US
dc.subjectThermodynamic functionsen_US
dc.subjectSurface and interface chemistryen_US
dc.subjectStatistical thermodynamicsen_US
dc.subjectIons and propertiesen_US
dc.titleLike-charge polymer-membrane complexation mediated by multivalent cations: one-loop-dressed strong coupling theoryen_US
dc.typeArticleen_US
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