Abstract
| Original language | Undefined |
|---|---|
| Pages (from-to) | 11474-1-11474-9 |
| Number of pages | 9 |
| Journal | Journal of chemical physics |
| Volume | 122 |
| Issue number | 11 |
| DOIs | |
| Publication status | Published - 2005 |
Keywords
- IR-51017
- METIS-223940
Cite this
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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 journal › Article › Academic › peer-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
Y1 - 2005
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.
KW - IR-51017
KW - METIS-223940
U2 - 10.1063/1.1861881
DO - 10.1063/1.1861881
M3 - Article
VL - 122
SP - 11474-1-11474-9
JO - Journal of chemical physics
JF - Journal of chemical physics
SN - 0021-9606
IS - 11
ER -