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Monitoring one-electron photo-oxidation of guanine in DNA crystals using ultrafast infrared spectroscopy

Hall, J. P., Poynton, F. E., Keane, P. M., Gurung, S. P., Brazier, J. A., Cardin, D. J., Winter, G., Gunnlaugsson, T., Sazanovich, I. V., Towrie, M., Cardin, C. J., Kelly, J. M. and Quinn, S. J. (2015) Monitoring one-electron photo-oxidation of guanine in DNA crystals using ultrafast infrared spectroscopy. Nature Chemistry, 7. pp. 961-967. ISSN 1755-4330

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To link to this item DOI: 10.1038/nchem.2369

Abstract/Summary

To understand the molecular origins of diseases caused by ultraviolet and visible light, and also to develop photodynamic therapy, it is important to resolve the mechanism of photoinduced DNA damage. Damage to DNA bound to a photosensitizer molecule frequently proceeds by one-electron photo-oxidation of guanine, but the precise dynamics of this process are sensitive to the location and the orientation of the photosensitizer, which are very difficult to define in solution. To overcome this, ultrafast time-resolved infrared (TRIR) spectroscopy was performed on photoexcited ruthenium polypyridyl–DNA crystals, the atomic structure of which was determined by X-ray crystallography. By combining the X-ray and TRIR data we are able to define both the geometry of the reaction site and the rates of individual steps in a reversible photoinduced electron-transfer process. This allows us to propose an individual guanine as the reaction site and, intriguingly, reveals that the dynamics in the crystal state are quite similar to those observed in the solvent medium.

Item Type:Article
Refereed:Yes
Divisions:Faculty of Life Sciences > School of Chemistry, Food and Pharmacy > Department of Chemistry
Interdisciplinary centres and themes > Chemical Analysis Facility (CAF) > NMR (CAF)
Interdisciplinary centres and themes > Chemical Analysis Facility (CAF) > Spectrometry (CAF)
Interdisciplinary centres and themes > Chemical Analysis Facility (CAF) > Xray (CAF)
Faculty of Life Sciences > School of Chemistry, Food and Pharmacy > School of Pharmacy > Medicinal Chemistry Research Group
ID Code:46101
Publisher:Nature Publishing Group

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