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Cryogenic Ion Fluorescence Spectroscopy: FRET in Rhodamine Homodimers and Heterodimers.

Christina Kjaer1, André Vu-Phung1, Thomas Toft Lindkvist1

  • 1Department of Physics and Astronomy, Aarhus University, Ny Munkegade 120, 8000, Aarhus C, Denmark.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|August 11, 2023
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Summary

This study demonstrates Förster Resonance Energy Transfer (FRET) in rhodamine dye dimers. Even in identical homodimers, selective excitation and energy transfer occur, revealing fundamental light-absorber communication.

Keywords:
FRETfluorescencemass spectroscopyrhodamine dimersstokes shift

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Area of Science:

  • Photophysics
  • Spectroscopy
  • Molecular interactions

Background:

  • Internal electronic communication in light-absorbers is crucial for energy transport.
  • Rhodamine dye dimers provide a model system to study these interactions.
  • Gas-phase studies eliminate solvent effects, maximizing charge-induced spectral shifts.

Purpose of the Study:

  • To investigate the intrinsic photophysics of rhodamine homodimers and heterodimers.
  • To understand energy transfer mechanisms in covalently linked dye systems.
  • To demonstrate Förster Resonance Energy Transfer (FRET) in homodimers.

Main Methods:

  • Gas-phase experiments on frozen molecular ions at cryogenic temperatures.
  • Utilized the LUNA2 mass spectroscopy setup.
  • Measured absorption (fluorescence excitation) and dispersed-fluorescence spectra.

Main Results:

  • Observed redshifted absorption bands in dimers compared to monomers due to inter-dye electric fields.
  • Achieved selective excitation of individual dyes within homodimers at low temperatures.
  • Demonstrated dominant fluorescence emission from the lowest energy dye, irrespective of initial excitation.
  • Unambiguously showed FRET occurring in homodimers, with one dye acting as donor and the other as acceptor.

Conclusions:

  • Förster Resonance Energy Transfer is unequivocally demonstrated in rhodamine homodimers.
  • Selective excitation and energy transfer are possible even between chemically identical, closely linked dyes.
  • Gas-phase cryogenic spectroscopy provides unique insights into fundamental photophysical processes.