Revealing competitive Forster-type resonance energy-transfer pathways in single bichromophoric molecules

Proc Natl Acad Sci U S A. 2003 Nov 11;100(23):13146-51. doi: 10.1073/pnas.2235805100. Epub 2003 Oct 28.

Abstract

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 homo-energy 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.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Fluorescence Resonance Energy Transfer / methods*
  • Models, Chemical
  • Perylene / chemistry
  • Physical Phenomena
  • Physics
  • Polymers / chemistry
  • Spectrometry, Fluorescence / methods*
  • Time Factors

Substances

  • Polymers
  • Perylene