0000000000255644
AUTHOR
Rémi Métivier
Single-molecule spectroscopy of molecular aggregates at low temperature
We have conducted single-molecule spectroscopy of a fluorescent polyphenylene dendrimer consisting of four peripheral perylenemonoimides which serve as energy donors and a central terrylenediimide which is the energy acceptor. After selective excitation of the donors the low-temperature emission spectra of single dendrimers show the purely electronic zero-phonon line as the most prominent feature of the acceptor. These sharp emission lines are subjected to appreciable spectral shifts. Fluorescence excitation spectroscopy of individual dendrimers in the spectral region of the donor absorption allows to extract energy transfer rates for single donors within the dendrimer. Although the energy …
Electronic Excitation Energy Transfer between Two Single Molecules Embedded in a Polymer Host
Unidirectional electronic excitation energy transfer from a photoexcited donor chromophore to a ground state acceptor chromophore - both linked by a rigid bridge - has been investigated by low temperature high-resolution single molecule spectroscopy. Our approach allows for accurately accessing static disorder in the donor and acceptor electronic transitions and to calculate the spectral overlap for each couple. By plotting the experimentally determined transfer rates against the spectral overlap, we can distinguish and quantify Förster- and non-Förster-type contributions to the energy transfer.
Energy transfer rates and pathways of single donor chromophores in a multichromophoric dendrimer built around a central acceptor core.
An artificial light-harvesting dendrimer showing highly efficient electronic excitation energy transfer from four peripheral donors to one central acceptor has been investigated by single-molecule spectroscopy at low temperatures. Confocal imaging in combination with frequency selective excitation spectroscopy gives direct access to energy transfer rates of individual donors and allows the determination of energy transfer pathways within a single multichromophoric aggregate.
Intramolecular electronic excitation energy transfer in donor∕acceptor dyads studied by time and frequency resolved single molecule spectroscopy
Electronic excitation energy transfer has been studied by single molecule spectroscopy in donor/acceptor dyads composed of a perylenediimide donor and a terrylenediimide acceptor linked by oligo(phenylene) bridges of two different lengths. For the shorter bridge (three phenylene units) energy is transferred almost quantitatively from the donor to the acceptor, while for the longer bridge (seven phenylene units) energy transfer is less efficient as indicated by the occurrence of donor and acceptor emission. To determine energy transfer rates and efficiencies at the single molecule level, several methods have been employed. These comprise time-correlated single photon counting techniques at r…