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Direct Observation of Radical Intermediates in Protein-Dependent DNA Charge Transport

Wagenknecht, Hans-Achim and Rajski, Scott R. and Pascaly, Matthias and Stemp, Eric D. A. and Barton, Jacqueline K. (2001) Direct Observation of Radical Intermediates in Protein-Dependent DNA Charge Transport. Journal of the American Chemical Society, 123 (19). pp. 4400-4407. ISSN 0002-7863. https://resolver.caltech.edu/CaltechAUTHORS:20160208-144324209

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Abstract

Charge migration through the DNA base stack has been probed both spectroscopically, to observe the formation of radical intermediates, and biochemically, to assess irreversible oxidative DNA damage. Charge transport and radical trapping were examined in DNA assemblies in the presence of a site-specifically bound methyltransferase HhaI mutant and an intercalating ruthenium photooxidant using the flash-quench technique. The methyltransferase mutant, which can flip out a base and insert a tryptophan side chain within the DNA cavity, is found to activate long-range hole transfer through the base pair stack. Protein-dependent DNA charge transport is observed over 50 Å with guanine radicals formed >10^6 s^(-1); hole transport through DNA over this distance is not rate-limiting. Given the time scale and distance regime, such protein-dependent DNA charge transport chemistry requires consideration physiologically.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/ja003986lDOIArticle
http://pubs.acs.org/doi/abs/10.1021/ja003986lPublisherArticle
ORCID:
AuthorORCID
Barton, Jacqueline K.0000-0001-9883-1600
Additional Information:© 2001 American Chemical Society. Received November 16, 2000. Publication Date (Web): April 20, 2001. We are grateful to the NIH (GM49216 to J.K.B.) for financial support. We also thank the Deutsche Forschungsgemeinschaft (H.A.W.) the Deutscher Akademischer Austauschdienst (M.P.), and the American Cancer Society (S.R.R.) for postdoctoral fellowships and Mount St. Mary's College Professional Development Fund and NSF (MCB981-7338) for funding of E.D.A.S. We are also very grateful to Drs.S. Kumar and R. J. Roberts of New England Biolabs for wild-type and Q237W mutant M·HhaI.
Funders:
Funding AgencyGrant Number
NIHGM49216
Deutsche Forschungsgemeinschaft (DFG)UNSPECIFIED
Deutscher Akademischer Austauschdienst (DAAD)UNSPECIFIED
American Cancer SocietyUNSPECIFIED
Mount St. Mary's CollegeUNSPECIFIED
NSFMCB-9817338
Issue or Number:19
Record Number:CaltechAUTHORS:20160208-144324209
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20160208-144324209
Official Citation:Direct Observation of Radical Intermediates in Protein-Dependent DNA Charge Transport Hans-Achim Wagenknecht,Scott R. Rajski,Matthias Pascaly,Eric D. A. Stemp,† and, and Jacqueline K. Barton* Journal of the American Chemical Society 2001 123 (19), 4400-4407 DOI: 10.1021/ja003986l
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:64314
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:08 Feb 2016 23:34
Last Modified:03 Oct 2019 09:36

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