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    Dye Diffusion at Surfaces: Charge Matters
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    Department of Chemistry, Rice University, Houston, Texas 77251
    *Corresponding author. E-mail: [email protected]
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    Langmuir

    Cite this: Langmuir 2010, 26, 7, 4807–4812
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    https://doi.org/10.1021/la904749z
    Published February 17, 2010
    Copyright © 2010 American Chemical Society
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    Abstract

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    Fluorescence correlation spectroscopy and single molecule burst analysis were used to measure the effects of glass surface interactions on the diffusion of two common fluorescent dyes, one cationic and one anionic. The effects of dye−surface interactions on measured diffusion rates as a function of distance from the surface were investigated. Use of a three-axis piezo stage, combined with reference calibration measurements, enabled the accurate acquisition of surface-distance-dependent transport data. This analysis reveals attractive interactions between the cationic dye and the surface, which significantly alter the extracted diffusion values and persist in the measurements up to 1.0 μm from the surface. The Coulomb attraction between the cationic dye and the surface also results in rare, long-lived association events that lead to irreproducibility in extracted diffusion values. In addition to an assignment of the association lifetime for these events, this paper demonstrates that, if experiments must be performed with cationic probes near a glass surface, the use of solution electrolytes can eliminate deleterious dye−surface interactions, as the dyes were tested in a variety of environments. Finally, our data demonstrate that a better dye choice is an anionic probe, which exhibits no depth dependence of diffusion characteristics above a glass surface.

    Copyright © 2010 American Chemical Society

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    Supporting Information

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    Autocorrelation curves for Rhodamine 6G (Figure S1) and Alexa 555 (Figure S2); single molecular blip frequency analysis in acidic conditions (Figure S3). This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cited By

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    Langmuir

    Cite this: Langmuir 2010, 26, 7, 4807–4812
    Click to copy citationCitation copied!
    https://doi.org/10.1021/la904749z
    Published February 17, 2010
    Copyright © 2010 American Chemical Society
    Request reuse permissions

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