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Oxidative DNA damage through long-range electron transfer

D B Hall1, R E Holmlin, J K Barton

  • 1Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena 91125, USA.

Nature
|August 22, 1996
PubMed
Summary
This summary is machine-generated.

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DNA's pi-stack facilitates charge migration, enabling remote oxidative damage. This research shows DNA can transfer holes over distances, causing specific damage at guanine-guanine sites.

Area of Science:

  • Molecular Biology
  • Biophysics
  • Chemical Biology

Background:

  • The DNA double helix's pi-stacked base pairs have long been theorized as a pathway for charge migration.
  • Understanding charge mobility in DNA is crucial for comprehending DNA damage mechanisms.
  • Previous studies demonstrated DNA's role as a molecular bridge for photo-induced electron transfer.

Purpose of the Study:

  • To investigate the potential for DNA to mediate oxidative damage from a distance.
  • To evaluate the role of hole migration through the DNA pi-stack in promoting oxidative damage.
  • To identify specific DNA sequences susceptible to remote oxidative attack.

Main Methods:

  • Utilizing a rhodium metallointercalator to introduce photoexcited holes into DNA.

Related Experiment Videos

  • Synthesizing oligomeric DNA duplexes with the intercalator positioned near specific oxidation sites (5'-GG-3' doublets).
  • Measuring the distance and yield of oxidative damage induced by the photoexcited hole.

    • Main Results:

    • Rhodium-induced photo-oxidation specifically targeted the 5'-G in 5'-GG-3' doublets.
    • Oxidative damage was observed up to 37 Angstroms from the rhodium intercalation site.
    • Damage yield was sensitive to oxidation potential and pi-stacking interactions, but not distance.

    Conclusions:

    • The DNA pi-stack can facilitate hole migration, enabling oxidative damage to occur at remote sites.
    • This mechanism highlights a novel pathway for DNA damage initiation.
    • The findings have implications for understanding DNA repair and developing strategies against DNA damage.