Sensitivity of Ru(bpy)₂dppz²⁺ Luminescence to DNA Defects

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Abstract

The luminescent characteristics of Ru(bpy)₂dppz²⁺ (dppz = dipyrido[3,2-a:2′,3′-c]phenazine), a DNA light switch, were investigated in the presence of oligonucleotides containing single base mismatches or an abasic site. In water, the ruthenium luminescence is quenched, but, bound to well matched duplex DNA, the Ru complex luminesces. Here we show that with DNAs containing a defect, rac-, Δ-, and Λ-Ru(bpy)₂dppz²⁺ exhibit significant luminescent enhancements above that with well matched DNA. In the presence of a single base mismatch, large luminescent enhancements are evident for the Δ-Ru isomer; the Λ-isomer shows particularly high luminescence bound to an oligonucleotide containing an abasic site. Similar increases are not evident with two common DNA-binding organic fluorophores, ethidium bromide and TO-PRO-3. Titrations with hairpin oligonucleotides containing a variable mismatch site show correlation between the level of luminescent enhancement and the thermodynamic destabilization associated with the mismatch. This correlation is reminiscent of that found earlier for a bulky rhodium complex that binds mismatched DNA sites through metalloinsertion, where the complex binds the DNA from the minor groove side, ejecting the mismatched bases into the major groove. Differential quenching studies with minor and major groove quenchers and time-resolved emission studies support this metalloinsertion mode for the dppz complex at the defect site. Certainly these data underscore the utility of Ru(bpy)₂dppz²⁺ as a sensitive luminescent reporter of DNA and its defects.

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This article has been cited by 5 ACS Journal articles (5 most recent appear below).

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    Molecules that selectively recognize DNA mismatches (MMs) play a key role as nucleic acids probes and as chemotherapeutic agents. Metallo-insertors bind to the minor groove (mG) of double strand (ds) DNA, expelling the mismatched base pairs and acting as ...

    Abstract | Full Text HTML | Hi-Res PDF | PDF w/ Links
• 

  New Heteroleptic Bis-Phenanthroline Copper(I) Complexes with Dipyridophenazine or Imidazole Fused Phenanthroline Ligands: Spectral, Electrochemical, and Quantum Chemical Studies

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    Two new sterically challenged diimine ligands L1 (2,9-dimesityl-2-(4′-bromophenyl)imidazo[4,5-f][1,10]phenanthroline) and L2 (3,6-di-n-butyl-11-bromodipyrido[3,2-a:2′,3′-c]phenazine) have been synthesized with the aim to build original heteroleptic copper(...

    Abstract | Full Text HTML | Hi-Res PDF | PDF w/ Links
• 

  EXAFS, DFT, Light-Induced Nucleobase Binding, and Cytotoxicity of the Photoactive Complex cis-[Ru(bpy)₂(CO)Cl]⁺

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  • EXAFS, DFT, Light-Induced Nucleobase Binding, and Cytotoxicity of the Photoactive Complex cis-[Ru(bpy)₂(CO)Cl]⁺

    Luca Salassa, Tiziana Ruiu, Claudio Garino, Ana M. Pizarro, Fabrizio Bardelli, Diego Gianolio, Aron Westendorf, Patrick J. Bednarski, Carlo Lamberti, Roberto Gobetto, and Peter J. Sadler
    Organometallics2010 29 (24), 6703-6710

    The aqueous photochemistry of cis-[Ru(bpy)2(CO)Cl]+ (1) was investigated at 310 K and under visible light (white) irradiation by NMR and ESI-HR-MS. Complex 1 releases a Cl ligand, coordinates a solvent molecule, and forms the complex cis-[Ru(bpy)2(CO)(H2O)...

    Abstract | Full Text HTML | Hi-Res PDF | PDF w/ Links
• 

  Modulating the Light Switch by ³MLCT-³ππ* State Interconversion

  Brigitte R. Spencer, Brian J. Kraft, Chris G. Hughes, Maren Pink, and Jeffrey M. Zaleski
  Inorganic Chemistry2010 49 (24), 11333-11345

  • Modulating the Light Switch by ³MLCT-³ππ* State Interconversion

    Brigitte R. Spencer, Brian J. Kraft, Chris G. Hughes, Maren Pink, and Jeffrey M. Zaleski
    Inorganic Chemistry2010 49 (24), 11333-11345

    The spectroscopic, electronic, and DNA-binding characteristics of two novel ruthenium complexes based on the dialkynyl ligands 2,3-bis(phenylethynyl)-1,4,8,9-tetraaza-triphenylene (bptt, 1) and 2,3-bis(4-tert-butyl-phenylethynyl)-1,4,8,9-tetraaza-...

    Abstract | Full Text HTML | Hi-Res PDF | PDF w/ Links
• 

  [Ru(bpy)₂dppz]²⁺ Electrochemiluminescence Switch and Its Applications for DNA Interaction Study and Label-free ATP Aptasensor

  Lianzhe Hu, Zheng Bian, Haijuan Li, Shuang Han, Yali Yuan, Lianxun Gao and Guobao Xu
  Analytical Chemistry2009 81 (23), 9807-9811

  • [Ru(bpy)₂dppz]²⁺ Electrochemiluminescence Switch and Its Applications for DNA Interaction Study and Label-free ATP Aptasensor

    Lianzhe Hu, Zheng Bian, Haijuan Li, Shuang Han, Yali Yuan, Lianxun Gao and Guobao Xu
    Analytical Chemistry2009 81 (23), 9807-9811

    [Ru(bpy)2dppz]2+ electrochemiluminescence (ECL) was studied, and it was used to investigate DNA interaction and develop a label-free ATP aptasensor for the first time. ECL of [Ru(bpy)2dppz]2+ is negligible in aqueous solution, and increases 1000 times ...

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