NDLI: Base pair motions control the rates and distance dependencies of reductive and oxidative DNA charge transfer

Content Provider	PubMed Central
Author	Valis, Linda Wang, Qiang Raytchev, Milen Ivan, Buchvarov Wagenknecht, Hans-achim Fiebig, Torsten
Copyright Year	2006
Abstract	In 1999, Wan et al. [Proc. Natl. Acad. Sci. USA 96, 6014–6019] published a pioneering paper that established the entanglement between DNA base pair motions and the transfer time of the charge carrier. The DNA assemblies contained an ethidium covalently bound via a flexible alkyl chain to the 5′ hydroxyl group of the DNA backbone. Although covalently attached, the loose way in which the ethidium was linked to DNA allowed for large degrees of conformational freedom and thus raised some concern with respect to conformational inhomogeneity. In this letter, we report studies on a different set of ethidium DNA conjugates. In contrast to the “Caltech systems,” these conjugates contain ethidium tightly incorporated (as a base pair surrogate) into the DNA base stack, opposite to an abasic site analog. Despite the tight binding, we found that charge transfer from the photoexcited ethidium base pair surrogate across two or more base pairs is several orders of magnitude slower than in case of the DNA systems bearing the tethered ethidium. To further broaden the scope of this account, we compared (oxidative) electron hole transfer and (reductive) electron transfer using the same ethidium chromophore as a charge donor in combination with two different charge acceptors. We found that both electron and hole transfer are characterized by similar rates and distance dependencies. The results demonstrate the importance of nuclear motions and conformational flexibility and underline the presence of a base gating mechanism, which appears to be generic to electronic transfer processes through π-stacked nucleic acids.
Related Links	http://dx.doi.org/10.1073/pnas.0600957103
Ending Page	10195
Page Count	4
Starting Page	10192
File Format	PDF
ISSN	00278424
e-ISSN	10916490
Journal	Proceedings of the National Academy of Sciences of the United States of America
Issue Number	27
Volume Number	103
Language	English
Publisher	National Academy of Sciences
Publisher Date	2006-07-05
Access Restriction	Open
Rights Holder	National Academy of Sciences
Subject Keyword	General Research in Higher Education
Content Type	Text
Resource Type	Article
Subject	Multidisciplinary

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