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Modulating the light switch by (3)MLCT-(3)ππ* state interconversion.

Brigitte R Spencer1, Brian J Kraft, Chris G Hughes

  • 1Department of Chemistry and Molecular Structure Center, Indiana University, Bloomington, Indiana 47405, United States.

Inorganic Chemistry
|November 25, 2010
PubMed
Summary

Ruthenium complexes with dialkynyl ligands were studied for their DNA-binding properties. One complex, [Ru(phen)(2)bptt](2+), shows significant luminescence enhancement upon binding to DNA, indicating intercalation.

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Area of Science:

  • Coordination Chemistry
  • Photophysics
  • Biophysical Chemistry

Background:

  • Ruthenium complexes are investigated for their potential in various applications, including photodynamic therapy and DNA sensing.
  • Dialkynyl ligands offer unique electronic and structural properties for tuning metal complex behavior.

Purpose of the Study:

  • To synthesize and characterize novel ruthenium complexes with dialkynyl ligands: 2,3-bis(phenylethynyl)-1,4,8,9-tetraaza-triphenylene (bptt) and 2,3-bis(4-tert-butyl-phenylethynyl)-1,4,8,9-tetraaza-triphenylene (tbptt).
  • To investigate the spectroscopic, electronic, and DNA-binding characteristics of these complexes.
  • To explore their potential as DNA intercalating agents and luminescence probes.

Main Methods:

  • Spectroscopic analysis (UV-Vis absorption, luminescence spectroscopy).
  • Electronic structure calculations.
  • DNA binding studies using luminescence titration.
  • Photophysical measurements (quantum yields, decay kinetics).

Main Results:

  • The electronic structure calculations revealed localization of frontier molecular orbitals on the pyrazine-dialkynyl portion of the free ligands.
  • Ruthenium complexes [Ru(phen)(2)bptt](2+) (3) and [Ru(phen)(2)tbptt](2+) (4) exhibited metal-to-ligand charge transfer (MLCT) transitions around 450 nm.
  • Complex 3 showed a significant increase in luminescence quantum yield upon addition of CT-DNA, indicating intercalation (K(b) = 3.3 × 10(4) M(-1)).
  • Complex 4, with tert-butyl substitution, displayed limited DNA binding and luminescence changes, suggesting inhibited intercalation.

Conclusions:

  • The study successfully synthesized and characterized novel ruthenium-dialkynyl complexes.
  • The tert-butyl substitution on the tbptt ligand hinders DNA intercalation, unlike the unsubstituted bptt ligand.
  • Complex 3 acts as a DNA light-switch complex, with its luminescence intensity modulated by DNA binding through intercalation, driven by competing MLCT and ππ* excited states.