Charge-Dependent Transport Switching of Single Molecular Ions in a Weak Polyelectrolyte Multilayer

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dc.citation.firstpage8391
dc.citation.issueNumber28
dc.citation.journalTitleLangmuir
dc.citation.lastpage8399
dc.citation.volumeNumber30
dc.contributor.authorTauzin, Lawrence J.
dc.contributor.authorShuang, Bo
dc.contributor.authorKisley, Lydia
dc.contributor.authorMansur, Andrea P.
dc.contributor.authorChen, Jixin
dc.contributor.authorde Leon, Al
dc.contributor.authorAdvincula, Rigoberto C.
dc.contributor.authorLandes, Christy F.
dc.date.accessioned2015-07-10T15:47:00Z
dc.date.available2015-07-10T15:47:00Z
dc.date.issued2014
dc.description.abstractThe tunable nature of weak polyelectrolyte multilayers makes them ideal candidates for drug loading and delivery, water filtration, and separations, yet the lateral transport of charged molecules in these systems remains largely unexplored at the single molecule level. We report the direct measurement of the charge-dependent, pH-tunable, multimodal interaction of single charged molecules with a weak polyelectrolyte multilayer thin film, a 10 bilayer film of poly(acrylic acid) and poly(allylamine hydrochloride) PAA/PAH. Using fluorescence microscopy and single-molecule tracking, two modes of interaction were detected: (1) adsorption, characterized by the molecule remaining immobilized in a subresolution region and (2) diffusion trajectories characteristic of hopping (D ∼ 10–9 cm2/s). Radius of gyration evolution analysis and comparison with simulated trajectories confirmed the coexistence of the two transport modes in the same single molecule trajectories. A mechanistic explanation for the probe and condition mediated dynamics is proposed based on a combination of electrostatics and a reversible, pH-induced alteration of the nanoscopic structure of the film. Our results are in good agreement with ensemble studies conducted on similar films, confirm a previously-unobserved hopping mechanism for charged molecules in polyelectrolyte multilayers, and demonstrate that single molecule spectroscopy can offer mechanistic insight into the role of electrostatics and nanoscale tunability of transport in weak polyelectrolyte multilayers.
dc.identifier.citationTauzin, Lawrence J., Shuang, Bo, Kisley, Lydia, et al.. "Charge-Dependent Transport Switching of Single Molecular Ions in a Weak Polyelectrolyte Multilayer." <i>Langmuir,</i> 30, no. 28 (2014) American Chemical Society: 8391-8399. http://dx.doi.org/10.1021/la5012007.
dc.identifier.doihttp://dx.doi.org/10.1021/la5012007
dc.identifier.urihttps://hdl.handle.net/1911/80880
dc.language.isoeng
dc.publisherAmerican Chemical Society
dc.rightsArticle is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
dc.titleCharge-Dependent Transport Switching of Single Molecular Ions in a Weak Polyelectrolyte Multilayer
dc.typeJournal article
dc.type.dcmiText
dc.type.publicationpublisher version
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