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

Lawrence J. Tauzin, Bo Shuang, Lydia Kisley, Andrea P. Mansur, Jixin Chen, Al De Leon, Rigoberto C. Advincula, Christy F. Landes

Research output: Contribution to journalArticle

16 Citations (Scopus)

Abstract

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 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.

Original languageEnglish
Pages (from-to)8391-8399
Number of pages9
JournalLangmuir
Volume30
Issue number28
DOIs
Publication statusPublished - 2014 Jul 22
Externally publishedYes

Fingerprint

Polyelectrolytes
molecular ions
Multilayers
Ions
Molecules
molecules
Trajectories
trajectories
Electrostatics
Water filtration
electrostatics
Fluorescence microscopy
Multilayer films
gyration
hydrochlorides
acrylic acid
polycyclic aromatic hydrocarbons
Polycyclic aromatic hydrocarbons
Acrylics
delivery

ASJC Scopus subject areas

  • Materials Science(all)
  • Condensed Matter Physics
  • Surfaces and Interfaces
  • Spectroscopy
  • Electrochemistry

Cite this

Tauzin, L. J., Shuang, B., Kisley, L., Mansur, A. P., Chen, J., De Leon, A., ... Landes, C. F. (2014). Charge-dependent transport switching of single molecular ions in a weak polyelectrolyte multilayer. Langmuir, 30(28), 8391-8399. https://doi.org/10.1021/la5012007

Charge-dependent transport switching of single molecular ions in a weak polyelectrolyte multilayer. / Tauzin, Lawrence J.; Shuang, Bo; Kisley, Lydia; Mansur, Andrea P.; Chen, Jixin; De Leon, Al; Advincula, Rigoberto C.; Landes, Christy F.

In: Langmuir, Vol. 30, No. 28, 22.07.2014, p. 8391-8399.

Research output: Contribution to journalArticle

Tauzin, LJ, Shuang, B, Kisley, L, Mansur, AP, Chen, J, De Leon, A, Advincula, RC & Landes, CF 2014, 'Charge-dependent transport switching of single molecular ions in a weak polyelectrolyte multilayer', Langmuir, vol. 30, no. 28, pp. 8391-8399. https://doi.org/10.1021/la5012007
Tauzin LJ, Shuang B, Kisley L, Mansur AP, Chen J, De Leon A et al. Charge-dependent transport switching of single molecular ions in a weak polyelectrolyte multilayer. Langmuir. 2014 Jul 22;30(28):8391-8399. https://doi.org/10.1021/la5012007
Tauzin, Lawrence J. ; Shuang, Bo ; Kisley, Lydia ; Mansur, Andrea P. ; Chen, Jixin ; De Leon, Al ; Advincula, Rigoberto C. ; Landes, Christy F. / Charge-dependent transport switching of single molecular ions in a weak polyelectrolyte multilayer. In: Langmuir. 2014 ; Vol. 30, No. 28. pp. 8391-8399.
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