Fluorescence Lifetime Fluctuations of Single Molecules Probe Local Density Fluctuations in Disordered Media: A Bulk Approach

R.A.L. Vallée, N. Tomczak, Gyula J. Vancso, L. Kuipers, N.F. van Hulst

Research output: Contribution to journalArticleAcademicpeer-review

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Abstract

We investigated the nanometer scale mobility of polymers in the glassy state by monitoring the dynamics of embedded single fluorophores. Recently we reported on fluorescence lifetime fluctuations which reflect the segmental rearrangement dynamics of the polymer in the surroundings of the single molecule probe. Here we focus on the nature of these fluorescence lifetime fluctuations. First the potential role of quenching and molecular conformational changes is discussed. Next we concentrate on the influence of the radiative density of states on the spontaneous emission of individual dye molecules embedded in a polymer. To this end we present a theory connecting the effective-medium theory to a cell-hole model, originating from the Simha¿Somcynsky free-volume theory. The relation between the derived distributions of free volume and fluorescence lifetime allows one to determine the number of segments involved in the local rearrangement directly from experimental data. Results for two different polymers as a function of temperature are presented.
Original languageUndefined
Pages (from-to)11474-1-11474-9
Number of pages9
JournalJournal of chemical physics
Volume122
Issue number11
DOIs
Publication statusPublished - 2005

Keywords

  • IR-51017
  • METIS-223940

Cite this

Vallée, R.A.L. ; Tomczak, N. ; Vancso, Gyula J. ; Kuipers, L. ; van Hulst, N.F. / Fluorescence Lifetime Fluctuations of Single Molecules Probe Local Density Fluctuations in Disordered Media: A Bulk Approach. In: Journal of chemical physics. 2005 ; Vol. 122, No. 11. pp. 11474-1-11474-9.
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abstract = "We investigated the nanometer scale mobility of polymers in the glassy state by monitoring the dynamics of embedded single fluorophores. Recently we reported on fluorescence lifetime fluctuations which reflect the segmental rearrangement dynamics of the polymer in the surroundings of the single molecule probe. Here we focus on the nature of these fluorescence lifetime fluctuations. First the potential role of quenching and molecular conformational changes is discussed. Next we concentrate on the influence of the radiative density of states on the spontaneous emission of individual dye molecules embedded in a polymer. To this end we present a theory connecting the effective-medium theory to a cell-hole model, originating from the Simha¿Somcynsky free-volume theory. The relation between the derived distributions of free volume and fluorescence lifetime allows one to determine the number of segments involved in the local rearrangement directly from experimental data. Results for two different polymers as a function of temperature are presented.",
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Fluorescence Lifetime Fluctuations of Single Molecules Probe Local Density Fluctuations in Disordered Media: A Bulk Approach. / Vallée, R.A.L.; Tomczak, N.; Vancso, Gyula J.; Kuipers, L.; van Hulst, N.F.

In: Journal of chemical physics, Vol. 122, No. 11, 2005, p. 11474-1-11474-9.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Fluorescence Lifetime Fluctuations of Single Molecules Probe Local Density Fluctuations in Disordered Media: A Bulk Approach

AU - Vallée, R.A.L.

AU - Tomczak, N.

AU - Vancso, Gyula J.

AU - Kuipers, L.

AU - van Hulst, N.F.

PY - 2005

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N2 - We investigated the nanometer scale mobility of polymers in the glassy state by monitoring the dynamics of embedded single fluorophores. Recently we reported on fluorescence lifetime fluctuations which reflect the segmental rearrangement dynamics of the polymer in the surroundings of the single molecule probe. Here we focus on the nature of these fluorescence lifetime fluctuations. First the potential role of quenching and molecular conformational changes is discussed. Next we concentrate on the influence of the radiative density of states on the spontaneous emission of individual dye molecules embedded in a polymer. To this end we present a theory connecting the effective-medium theory to a cell-hole model, originating from the Simha¿Somcynsky free-volume theory. The relation between the derived distributions of free volume and fluorescence lifetime allows one to determine the number of segments involved in the local rearrangement directly from experimental data. Results for two different polymers as a function of temperature are presented.

AB - We investigated the nanometer scale mobility of polymers in the glassy state by monitoring the dynamics of embedded single fluorophores. Recently we reported on fluorescence lifetime fluctuations which reflect the segmental rearrangement dynamics of the polymer in the surroundings of the single molecule probe. Here we focus on the nature of these fluorescence lifetime fluctuations. First the potential role of quenching and molecular conformational changes is discussed. Next we concentrate on the influence of the radiative density of states on the spontaneous emission of individual dye molecules embedded in a polymer. To this end we present a theory connecting the effective-medium theory to a cell-hole model, originating from the Simha¿Somcynsky free-volume theory. The relation between the derived distributions of free volume and fluorescence lifetime allows one to determine the number of segments involved in the local rearrangement directly from experimental data. Results for two different polymers as a function of temperature are presented.

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KW - METIS-223940

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