CdSe/ZnS Nanocrystals with Dye-Functionalized Polymer Ligands Containing Many Anchor Groups

Coherent Electronic Coupling versus Localization in Individual Molecular Dimers

International audience; The electronic excitation transfer and coherent electronic coupling strength were investigated in molecular dimers by spectrally resolved confocal fluorescence spectroscopy. The direct probe of electronic coupling strength distribution was possible due to static disorder in polymer host by single molecule measurements. The dimers with delocalized excitation were also found in comparison to emission originated from localized states. The delocalized and localized state transitions were observed for dimers which were attributed to structural fluctuations of guest-host system.

Photon antibunching and collective effects in the fluorescence of single bichromophoric molecules.

The fluorescence of individual pairs of perylenemonoimide chromophores coupled via a short rigid linker is investigated. Photon antibunching is reported, indicating collective effects in the fluorescence, which are further substantiated by the observation of collective triplet off times and triplet lifetime shortening. The experimental findings are analyzed in terms of singlet-singlet and singlet-triplet annihilation based on Forster type energy transfer. The results reported here demonstrate that the statistical properties of the emission light of isolated single quantum systems can serve as a hallmark of intermolecular interactions.

Three-dimensional orientational colocalization of individual donor--acceptor pairs.

We report on the determination of the three-dimensional orientation of the donor and acceptor transition dipoles in individual fluorescence resonance energy transfer (FRET) pairs by means of scanning optical microscopy with annular illumination. Knowledge of the mutual orientation of the donor and acceptor dipole is mandatory for reliable distance determination based on FRET efficiency measurements. In our model system perylenediimide as the donor and terryelenediimide as the acceptor are coupled via a stiff p-terphenyl linker. The absorption dipoles of the donor and acceptor are selectively addressed by the 488 nm and 647 line of an Ar/Kr mixed gas laser, respectively. A clear deviation fr…

Photoblinking and photobleaching of rylene diimide dyes.

We investigate photoblinking and photobleaching of perylene diimide (PDI) and its higher homologue terrylene diimide (TDI). Single molecule fluorescence trajectories of the dye molecules embedded in PMMA under ambient conditions exhibit "on"-"off" blinking in the time range from ms to s. Due to the limited statistics of individual trajectories we construct ensemble distributions of "on" and "off" times which follow power laws with similar power law coefficients (m(on) ≈ 1.18, m(off) ≈ 1.31). The blinking is attributed to reversible formation of radical cations which are presumably created by electron transfer from higher excited triplet states T(n) of the molecules to acceptor levels in the…

CdSe/ZnS-Nanokristalle mit farbstoffmarkierten Polymerliganden mit mehrfachen Ankergruppen

Precision and accuracy of single-molecule FRET measurements-a multi-laboratory benchmark study

Single-molecule Forster resonance energy transfer (smFRET) is increasingly being used to determine distances, structures, and dynamics of biomolecules in vitro and in vivo. However, generalized protocols and FRET standards to ensure the reproducibility and accuracy of measurements of FRET efficiencies are currently lacking. Here we report the results of a comparative blind study in which 20 labs determined the FRET efficiencies (E) of several dye-labeled DNA duplexes. Using a unified, straightforward method, we obtained FRET efficiencies with s.d. between +/- 0.02 and +/- 0.05. We suggest experimental and computational procedures for converting FRET efficiencies into accurate distances, and…

Optical Microscopy and Spectroscopy of Single Molecules