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Intramolecular electronic excitation energy transfer in donor∕acceptor dyads studied by time and frequency resolved single molecule spectroscopy
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10.1063/1.2841474
/content/aip/journal/jcp/128/12/10.1063/1.2841474
http://aip.metastore.ingenta.com/content/aip/journal/jcp/128/12/10.1063/1.2841474

Figures

Image of FIG. 1.
FIG. 1.

Absorption (black lines) and emission ensemble spectra (gray lines) of (a) PDI and TDI, (b) dyad 1 and (c) dyad 2. Each compound has been dissolved in toluene.

Image of FIG. 2.
FIG. 2.

Emission spectra of single dyads 1 and 2 embedded in PMMA at . In 2 intramolecular energy transfer is slow enough such that weak emission from the donor is observed .

Image of FIG. 3.
FIG. 3.

Fluorescence time trace of the same single dyad 2 at , the emission spectrum of which is shown in Fig. 2. After PDI bleached first, seen in the drop of the intensity. The corresponding rise∕decay time profiles before and after bleaching are shown in the inset. The profiles consist of before and counts after bleaching of PDI. The difference shown in the upper part of the inset originates from the energy transfer (Ref. 31).

Image of FIG. 4.
FIG. 4.

Distribution of single molecule EET rates of dyad 2, obtained at room temperature. The open bars represent the rates determined from the rise∕decay time profiles, while the filled bars are calculated according to Förster theory from spectral overlaps, each on a single molecule level. The solid lines show a simulated rate distribution originating solely from different molecular conformations. This distribution has been scaled to fit both histograms. For more details see text.

Image of FIG. 5.
FIG. 5.

Inhomogeneous distributions of electronic transition frequencies from dyads 1 and 2, for both donor (PDI) and acceptor (TDI). At the distributions of purely electronic zero-phonon lines are plotted [(a) and (b)] while at room temperature (c) the distributions of emission maxima are shown. The bold lines are Gaussians fitted to the inhomogeneous distributions.

Image of FIG. 6.
FIG. 6.

Emission spectra of single dyads 1 (a) and 2 (b) embedded in PMMA at low temperature (, ). In 1 energy transfer is so fast that no donor emission is visible.

Image of FIG. 7.
FIG. 7.

Emission spectra from a single dyad 2, taken at . Spectral shifts which are stronger for PDI lead to variations in the ratio , which nicely correlates to the estimated spectral overlaps, .

Image of FIG. 8.
FIG. 8.

Distribution of single molecule EET rates of dyad 1 obtained at . The open bars represent the rates determined from donor (PDI) excitation spectra, while the filled bars are calculated from the spectral overlaps according to Förster theory. The solid lines show a simulated rate distribution solely originating from different molecular conformations. This distribution has been scaled to fit both histograms.

Image of FIG. 9.
FIG. 9.

Experimentally determined energy transfer rates plotted vs the calculated spectral overlaps, see text. (Dyad , dyad 2: room temperature). The solid lines have been calculated according to Förster theory [Eq. (1)]. The dashed lines represent linear fits to the data.

Image of FIG. 10.
FIG. 10.

Spectral overlap between single molecule emission (PDI) and absorption (TDI) spectra at (sharp lines) and at room temperature. For better visibility the intensities of the room temperature spectra are enlarged five times. For more details see text.

Image of FIG. 11.
FIG. 11.

Comparison of transfer rate distributions at room temperature (RT) and (low temperature, LT) calculated within Förster theory. The calculation is based on the experimentally observed inhomogeneous distributions of dyad 1 at [Fig. 5(a)].

Image of Scheme 1.
Scheme 1.

Chemical structures of the donor∕acceptor dyads 1 and 2.

Tables

Generic image for table
Table I.

Summary of EET and molecular parameters for dyads 1 and 2.

Generic image for table
Table II.

Parameters of the fitted distributions as plotted in Fig. 5.

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/content/aip/journal/jcp/128/12/10.1063/1.2841474
2008-03-31
2014-04-18
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Intramolecular electronic excitation energy transfer in donor∕acceptor dyads studied by time and frequency resolved single molecule spectroscopy
http://aip.metastore.ingenta.com/content/aip/journal/jcp/128/12/10.1063/1.2841474
10.1063/1.2841474
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