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

dc.citation.firstpage8391en_US
dc.citation.issueNumber28en_US
dc.citation.journalTitleLangmuiren_US
dc.citation.lastpage8399en_US
dc.citation.volumeNumber30en_US
dc.contributor.authorTauzin, Lawrence J.en_US
dc.contributor.authorShuang, Boen_US
dc.contributor.authorKisley, Lydiaen_US
dc.contributor.authorMansur, Andrea P.en_US
dc.contributor.authorChen, Jixinen_US
dc.contributor.authorde Leon, Alen_US
dc.contributor.authorAdvincula, Rigoberto C.en_US
dc.contributor.authorLandes, Christy F.en_US
dc.date.accessioned2015-07-10T15:47:00Zen_US
dc.date.available2015-07-10T15:47:00Zen_US
dc.date.issued2014en_US
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.en_US
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.en_US
dc.identifier.doihttp://dx.doi.org/10.1021/la5012007en_US
dc.identifier.urihttps://hdl.handle.net/1911/80880en_US
dc.language.isoengen_US
dc.publisherAmerican Chemical Societyen_US
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.en_US
dc.titleCharge-Dependent Transport Switching of Single Molecular Ions in a Weak Polyelectrolyte Multilayeren_US
dc.typeJournal articleen_US
dc.type.dcmiTexten_US
dc.type.publicationpublisher versionen_US
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