Charge equilibration between two distinct sites in double helical DNA

Proceedings of the National Academy of Sciences of the United States of America
Sarah DelaneyJ K Barton

Abstract

DNA assemblies containing a pendant dipyridophenazine complex of Ru(II) along with two oxidative traps, a site containing the nucleoside analog methylindole (5'-GMG-3') and a 5'-GGG-3' site, have been constructed to explore long-range charge transport through the base pair stack. With these chemically well defined assemblies, in combination with the flash/quench technique, formation of the methylindole cation radical and the neutral guanine radical is monitored directly by using transient absorption spectroscopy, and yields of oxidative damage are quantitated biochemically by gel electrophoresis. In these assemblies the base radicals form with a rate of > or =10(7) s(-1). The rate of base radical formation does not change upon the addition of a second radical trap, the 5'-GGG-3' site; however, the yield of methylindole oxidation is significantly lower. This observation indicates that the 5'-GGG-3' site is effective in competing for the migrating charge and provides a second trapping site. Switching the orientation of the two trapping sites does not affect the yield of oxidized products at either site. Therefore, in DNA both forward and reverse charge transport occur so as to provide equilibration across the duplex on a timescal...Continue Reading

References

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Citations

Mar 11, 2010·Chemical Reviews·Joseph C Genereux, Jacqueline K Barton
Feb 14, 2006·Physical Chemistry Chemical Physics : PCCP·Tobias CramerThorsten Koslowski
Aug 2, 2012·Physical Chemistry Chemical Physics : PCCP·Natalie B MurenJacqueline K Barton
Jul 10, 2013·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Etienne GicquelPatricia Vicendo
Mar 2, 2005·Proceedings of the National Academy of Sciences of the United States of America·Eylon YavinJacqueline K Barton
Dec 18, 2004·Proceedings of the National Academy of Sciences of the United States of America·Fangwei ShaoJacqueline K Barton
Jan 1, 2013·Computational and Structural Biotechnology Journal·Ivan KanevWarren Sanger
Sep 27, 2005·Chemistry & Biology·Kiyohiko KawaiTetsuro Majima
Aug 30, 2005·Bioorganic & Medicinal Chemistry Letters·Kiyohiko KawaiTetsuro Majima
Jul 4, 2007·Angewandte Chemie·Katherine E AugustynJacqueline K Barton
Oct 31, 2008·Chemistry & Biodiversity·Vasil G BregadzeSophia Z Melikishvili
Aug 6, 2010·The Journal of Physical Chemistry. B·Kiyohiko KawaiTetsuro Majima
Feb 13, 2007·The Journal of Physical Chemistry. B·Kiyohiko KawaiTetsuro Majima

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