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Tuning Single-Molecule Dynamics in Functionalized Mesoporous Silica

Authors

  • Timo Lebold,

    1. Department of Chemistry and Biochemistry and Center for Nanoscience (CeNS), Ludwig-Maximilians-Universität München (LMU), Butenandtstrasse 5-13 (E), 81377 Munich (Germany), Fax: (+49) 89-2180-77622
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    • These authors contributed equally to this work.

  • Lea A. Mühlstein,

    1. Department of Chemistry and Biochemistry and Center for Nanoscience (CeNS), Ludwig-Maximilians-Universität München (LMU), Butenandtstrasse 5-13 (E), 81377 Munich (Germany), Fax: (+49) 89-2180-77622
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    • These authors contributed equally to this work.

  • Julia Blechinger,

    1. Department of Chemistry and Biochemistry and Center for Nanoscience (CeNS), Ludwig-Maximilians-Universität München (LMU), Butenandtstrasse 5-13 (E), 81377 Munich (Germany), Fax: (+49) 89-2180-77622
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  • Melanie Riederer,

    1. Department of Chemistry and Biochemistry and Center for Nanoscience (CeNS), Ludwig-Maximilians-Universität München (LMU), Butenandtstrasse 5-13 (E), 81377 Munich (Germany), Fax: (+49) 89-2180-77622
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  • Heinz Amenitsch Dr.,

    1. Institute of Biophysics and Nanosystems Research, Austrian Academy of Sciences, Schmiedlstrasse 6, 8042 Graz (Austria)
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  • Ralf Köhn Dr.,

    1. Department of Chemistry and Biochemistry and Center for Nanoscience (CeNS), Ludwig-Maximilians-Universität München (LMU), Butenandtstrasse 5-13 (E), 81377 Munich (Germany), Fax: (+49) 89-2180-77622
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  • Kalina Peneva,

    1. Max-Planck-Institute for Polymer Research, Ackermannweg 10, 55128 Mainz (Germany)
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  • Klaus Müllen Prof. Dr.,

    1. Max-Planck-Institute for Polymer Research, Ackermannweg 10, 55128 Mainz (Germany)
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  • Jens Michaelis Prof. Dr.,

    1. Department of Chemistry and Biochemistry and Center for Nanoscience (CeNS), Ludwig-Maximilians-Universität München (LMU), Butenandtstrasse 5-13 (E), 81377 Munich (Germany), Fax: (+49) 89-2180-77622
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  • Christoph Bräuchle Prof. Dr.,

    1. Department of Chemistry and Biochemistry and Center for Nanoscience (CeNS), Ludwig-Maximilians-Universität München (LMU), Butenandtstrasse 5-13 (E), 81377 Munich (Germany), Fax: (+49) 89-2180-77622
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  • Thomas Bein Prof. Dr.

    1. Department of Chemistry and Biochemistry and Center for Nanoscience (CeNS), Ludwig-Maximilians-Universität München (LMU), Butenandtstrasse 5-13 (E), 81377 Munich (Germany), Fax: (+49) 89-2180-77622
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Abstract

Diffusion of single molecules of a substituted terrylene diimide dye in functionalized mesoporous silica films was monitored by single-molecule fluorescence microscopy. By varying the chemical nature and density of the functional groups, the diffusion dynamics of the dye molecules can be controlled precisely. The picture shows a sketch of a dye molecule in a pore, diffusion data for different phenyl functionalization densities, and the trajectory of one molecule in a cyanopropyl-functionalized film.

original image

Mesoporous silica materials are promising host structures for diverse applications in nanoscience. Many applications can profit significantly from the ability to influence guest dynamics in the host matrix. To this end, we introduce covalently attached organic functionalization into the walls of mesoporous silica networks. Using single-molecule fluorescence microscopy, we study the diffusion behavior of single terrylene diimide dye molecules in functionalized mesoporous silica films. We show that, through variation of the chemical nature and density of the functional groups, the diffusion dynamics of the dye molecules, in the presence of the surfactant template, can be controlled precisely. The mean diffusion coefficient of the dye molecules increases or decreases depending on the functional group attached to the silica wall. This allows fine-tuning of the diffusion dynamics of the dye by approximately one order of magnitude. The observed changes in the mean diffusion coefficients can be explained by shielding of hydroxyl groups on the silica surface in combination with changes in the rigidity of the micellar packing in the film, as well as direct interactions between the functional groups and the dye molecules.

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