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Power-Law Blinking in the Fluorescence of Single Organic Molecules

Authors

  • Jacob P. Hoogenboom Dr.,

    1. Applied Optics Group, Faculty of Science & Technology and MESA+Institute for Nanotechnology, University of Twente, P.O. Box 217, 7500AE Enschede, The Netherlands, Fax: (+34) 935534000
    2. ICFO – Institut de Ciències Fotòniques, Av. del Canal Olímpic s/n, 08860 Castelldefels, Barcelona, Spain
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  • Jordi Hernando Dr.,

    1. Departament de Química, Universitat Autonóma de Barcelona UAB, Cerdanyola del Vallés, Spain
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  • Erik M. H. P. van Dijk Dr.,

    1. Applied Optics Group, Faculty of Science & Technology and MESA+Institute for Nanotechnology, University of Twente, P.O. Box 217, 7500AE Enschede, The Netherlands, Fax: (+34) 935534000
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  • Niek F. van Hulst Prof. Dr.,

    1. Applied Optics Group, Faculty of Science & Technology and MESA+Institute for Nanotechnology, University of Twente, P.O. Box 217, 7500AE Enschede, The Netherlands, Fax: (+34) 935534000
    2. ICFO – Institut de Ciències Fotòniques, Av. del Canal Olímpic s/n, 08860 Castelldefels, Barcelona, Spain
    3. ICREA-Institucío Catalana de Recerca i Estudis Avançats, 08015, Barcelona, Spain
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  • Maria F. García-Parajó Prof. Dr.

    1. Applied Optics Group, Faculty of Science & Technology and MESA+Institute for Nanotechnology, University of Twente, P.O. Box 217, 7500AE Enschede, The Netherlands, Fax: (+34) 935534000
    2. ICREA-Institucío Catalana de Recerca i Estudis Avançats, 08015, Barcelona, Spain
    3. Laboratory of NanoBioengineering, Parc Científic de Barcelona (PCB), Josep Samitier 1-5, 08028 Barcelona, Spain
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Abstract

The blinking behavior of perylene diïmide molecules is investigated at the single-molecule level. We observe long-time scale blinking of individual multi-chromophoric complexes embedded in a poly(methylmethacrylate) matrix, as well as for the monomeric dye absorbed on a glass substrate at ambient conditions. In both these different systems, the blinking of single molecules is found to obey analogous power-law statistics for both the on and off periods. The observed range for single-molecular power-law blinking extends over the full experimental time window, covering four orders of magnitude in time and six orders of magnitude in probability density. From molecule to molecule, we observe a large spread in off-time power-law exponents. The distributions of off-exponents in both systems are markedly different whereas both on-exponent distributions appear similar. Our results are consistent with models that ascribe the power-law behavior to charge separation and (environment-dependent) recombination by electron tunneling to a dynamic distribution of charge acceptors. As a consequence of power-law statistics, single molecule properties like the total number of emitted photons display non-ergodicity.

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