TY - JOUR
T1 - Revealing competitive Förster-type resonance energy-transfer pathways in single bichromophoric molecules
AU - Hofkens, Johan
AU - Cotlet, Mircea
AU - Vosch, Tom
AU - Tinnefeld, Philip
AU - Weston, Kenneth D.
AU - Ego, Christophe
AU - Grimsdale, Andrew
AU - Müllen, Klaus
AU - Beljonne, David
AU - Brédas, Jean Luc
AU - Jordens, Sven
AU - Schweitzer, Gerd
AU - Sauer, Markus
AU - De Schryver, Frans
PY - 2003/11/11
Y1 - 2003/11/11
N2 - We demonstrate measurements of the efficiency of competing Förster-type energy-transfer pathways in single bichromophoric systems by monitoring simultaneously the fluorescence intensity, fluorescence lifetime, and the number of independent emitters with time. Peryleneimide end-capped fluorene trimers, hexamers, and polymers with interchromophore distances of 3.4, 5.9, and on average 42 nm, respectively, served as bichromophoric systems. Because of different energy-transfer efficiencies, variations in the interchromophore distance enable the switching between homoenergy transfer (energy hopping), singlet-singlet annihilation, and singlet-triplet annihilation. The data suggest that similar energy-transfer pathways have to be considered in the analysis of single-molecule trajectories of donor/acceptor pairs as well as in natural and synthetic multichromophoric systems such as light-harvesting antennas, oligomeric fluorescent proteins, and dendrimers. Here we report selectively visualization of different energy-transfer pathways taking place between identical fluorophores in individual bichromophoric molecules.
AB - We demonstrate measurements of the efficiency of competing Förster-type energy-transfer pathways in single bichromophoric systems by monitoring simultaneously the fluorescence intensity, fluorescence lifetime, and the number of independent emitters with time. Peryleneimide end-capped fluorene trimers, hexamers, and polymers with interchromophore distances of 3.4, 5.9, and on average 42 nm, respectively, served as bichromophoric systems. Because of different energy-transfer efficiencies, variations in the interchromophore distance enable the switching between homoenergy transfer (energy hopping), singlet-singlet annihilation, and singlet-triplet annihilation. The data suggest that similar energy-transfer pathways have to be considered in the analysis of single-molecule trajectories of donor/acceptor pairs as well as in natural and synthetic multichromophoric systems such as light-harvesting antennas, oligomeric fluorescent proteins, and dendrimers. Here we report selectively visualization of different energy-transfer pathways taking place between identical fluorophores in individual bichromophoric molecules.
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U2 - 10.1073/pnas.2235805100
DO - 10.1073/pnas.2235805100
M3 - Article
C2 - 14583594
AN - SCOPUS:0345687198
SN - 0027-8424
VL - 100
SP - 13146
EP - 13151
JO - Proceedings of the National Academy of Sciences of the United States of America
JF - Proceedings of the National Academy of Sciences of the United States of America
IS - 23
ER -