Charge-dependent transport switching of single molecular ions in a weak polyelectrolyte multilayer

The 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 measureme...

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Veröffentlicht in:Langmuir : the ACS journal of surfaces and colloids. - 1992. - 30(2014), 28 vom: 22. Juli, Seite 8391-9
1. Verfasser: Tauzin, Lawrence J (VerfasserIn)
Weitere Verfasser: Shuang, Bo, Kisley, Lydia, Mansur, Andrea P, Chen, Jixin, de Leon, Al, Advincula, Rigoberto C, Landes, Christy F
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2014
Zugriff auf das übergeordnete Werk:Langmuir : the ACS journal of surfaces and colloids
Schlagworte:Journal Article Research Support, N.I.H., Extramural Research Support, Non-U.S. Gov't Research Support, U.S. Gov't, Non-P.H.S. Acrylic Resins Ions Polymers carbopol 940 4Q93RCW27E
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245 1 0 |a Charge-dependent transport switching of single molecular ions in a weak polyelectrolyte multilayer 
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520 |a The 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) cm(2)/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 
650 4 |a Journal Article 
650 4 |a Research Support, N.I.H., Extramural 
650 4 |a Research Support, Non-U.S. Gov't 
650 4 |a Research Support, U.S. Gov't, Non-P.H.S. 
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650 7 |a Ions  |2 NLM 
650 7 |a Polymers  |2 NLM 
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700 1 |a Shuang, Bo  |e verfasserin  |4 aut 
700 1 |a Kisley, Lydia  |e verfasserin  |4 aut 
700 1 |a Mansur, Andrea P  |e verfasserin  |4 aut 
700 1 |a Chen, Jixin  |e verfasserin  |4 aut 
700 1 |a de Leon, Al  |e verfasserin  |4 aut 
700 1 |a Advincula, Rigoberto C  |e verfasserin  |4 aut 
700 1 |a Landes, Christy F  |e verfasserin  |4 aut 
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773 1 8 |g volume:30  |g year:2014  |g number:28  |g day:22  |g month:07  |g pages:8391-9 
856 4 0 |u http://dx.doi.org/10.1021/la5012007  |3 Volltext 
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