Single molecule spectroscopy reveals heterogeneous transport mechanisms for molecular ions in a polyelectrolyte polymer brush

Carmen Reznik, Nicel Estillore, Rigoberto C. Advincula, Christy F. Landes

Research output: Contribution to journalArticle

26 Citations (Scopus)

Abstract

Single molecule polarization and fluorescence correlation spectroscopy were used to evaluate heterogeneous transport mechanisms of molecular ions within supported polyelectrolyte brushes. Modes of diffusive transport include periods of significantly restricted rotational motion, often maintained over tens of milliseconds; periods of fast molecular rotation; and occasional adsorption of fluorescent probe molecules in the brush. The studies reveal rapid switching between orientational states during each observed mode of motion. Through quantitative analysis of state occupation times, the rate constants for transitions from weakly associated to strongly associated states were extracted. Additionally, the pH dependence of the ion transport rates in the brush exhibits an abrupt, rather than continuous, trend. These single molecule studies demonstrate the presence of dynamic anisotropic interactions between the charged molecular probe and the polymer brush and provide experimental evidence of stimuli responsive switchable transport functionality in the polyelectrolyte brush.

Original languageEnglish
Pages (from-to)14611-14618
Number of pages8
JournalJournal of Physical Chemistry B
Volume113
Issue number44
DOIs
Publication statusPublished - 2009 May 11
Externally publishedYes

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brushes
Brushes
Polyelectrolytes
molecular ions
Polymers
Spectroscopy
Ions
Molecular Probes
Molecules
Fluorescence Spectrometry
Ion Transport
polymers
Fluorescent Dyes
Occupations
spectroscopy
Adsorption
molecules
molecular rotation
probes
stimuli

ASJC Scopus subject areas

  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry
  • Materials Chemistry

Cite this

Single molecule spectroscopy reveals heterogeneous transport mechanisms for molecular ions in a polyelectrolyte polymer brush. / Reznik, Carmen; Estillore, Nicel; Advincula, Rigoberto C.; Landes, Christy F.

In: Journal of Physical Chemistry B, Vol. 113, No. 44, 11.05.2009, p. 14611-14618.

Research output: Contribution to journalArticle

Reznik, Carmen ; Estillore, Nicel ; Advincula, Rigoberto C. ; Landes, Christy F. / Single molecule spectroscopy reveals heterogeneous transport mechanisms for molecular ions in a polyelectrolyte polymer brush. In: Journal of Physical Chemistry B. 2009 ; Vol. 113, No. 44. pp. 14611-14618.
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