Single molecule fluorescence microscopy investigations on heterogeneity of translational diffusion in thin polymer films

Bente M. I. Flier; Moritz Baier; Johannes Huber; Klaus Müllen; Stefan Mecking; Andreas Zumbusch; Dominik Wöll

doi:10.1039/C0CP01801E

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Physical Chemistry Chemical Physics

Issue 5, 2011

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Single molecule fluorescence microscopy investigations on heterogeneity of translational diffusion in thin polymer films

Bente M. I. Flier,^a Moritz Baier,^a Johannes Huber,^a Klaus Müllen,^b Stefan Mecking,^a Andreas Zumbusch^a and Dominik Wöll*^a^c

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Fachbereich Chemie, Universität Konstanz, Universitätsstrasse 10, 78464 Konstanz, Germany
E-mail: dominik.woell@uni-konstanz.de ;
Tel: +49 7531 88 2024

Max-Planck-Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany

Zukunftskolleg, Universität Konstanz, Universitätsstrasse 10, 78464 Konstanz, Germany

Phys. Chem. Chem. Phys., 2011,13, 1770-1775

DOI: 10.1039/C0CP01801E
Received 13 Sep 2010, Accepted 16 Nov 2010
First published online 10 Dec 2010

This article is part of themed collection: Single-molecule optical studies of soft and complex matter

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Abstract
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Translational diffusion of single perylene diimide molecules in 25 nm thin polymer films was investigated by single molecule widefield fluorescence microscopy. Spatial heterogeneities in single molecule motion were detected and analyzed by a new, quantitative method which draws a comparison of log-Gaussian fits of experimentally determined diffusion coefficient-distributions and diffusion coefficient-distributions from Monte Carlo random walk simulations. Heterogeneities could be observed close to the glass transition temperature, but disappear at ca. 1.1 × T_g. At higher temperatures, heterogeneities do not exist or they average out on the time and length scales of observation. The observed heterogeneities also explain why the dependency of diffusion coefficients on temperature does not follow Vogel–Fulcher–Tammann behavior.

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Bente M. I. Flier
Moritz Baier
Johannes Huber
Klaus Müllen
Stefan Mecking
Andreas Zumbusch
Dominik Wöll

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