DNA嵌入剂乙锭在水中的飞秒动力学以及与单核苷酸的电子转移。
Femtosecond dynamics of the DNA intercalator ethidium and electron transfer with mononucleotides in water.
作者信息
Fiebig T, Wan C, Kelley S O, Barton J K, Zewail A H
机构信息
Laboratory for Molecular Science, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology, Pasadena, CA 91125, USA.
出版信息
Proc Natl Acad Sci U S A. 1999 Feb 16;96(4):1187-92. doi: 10.1073/pnas.96.4.1187.
Abstract
Ethidium (E) is a powerful probe of DNA dynamics and DNA-mediated electron transfer (ET). Molecular dynamical processes, such as solvation and orientation, are important on the time scale of ET. Here, we report studies of the femtosecond and picosecond time-resolved dynamics of E, E with 2'deoxyguanosine triphosphate (GTP) in water, and E with 7-deaza-2'-deoxyguanosine triphosphate (ZTP) in water; E undergoes ET with ZTP but not GTP. These studies elucidate the critical role of relative orientational motions of the donor-acceptor complex on ET processes in solution. For ET from ZTP to E, such motions are in fact the rate-determining step. Our results indicate that these complexes reorient before ET. The time scale for the solvation of E in water is 1 ps, and the orientational relaxation time of E is 70 ps. The impact of orientational and solvation effects on ET between E and mononucleotides must be considered in the application of E as a probe of DNA ET.
摘要
溴化乙锭（E）是一种用于研究DNA动力学和DNA介导的电子转移（ET）的强大探针。分子动力学过程，如溶剂化和取向，在电子转移的时间尺度上很重要。在此，我们报告了对E、E与三磷酸2'-脱氧鸟苷（GTP）在水中以及E与三磷酸7-脱氮-2'-脱氧鸟苷（ZTP）在水中的飞秒和皮秒时间分辨动力学的研究；E与ZTP发生电子转移，但与GTP不发生。这些研究阐明了供体-受体复合物的相对取向运动在溶液中电子转移过程中的关键作用。对于从ZTP到E的电子转移，这种运动实际上是速率决定步骤。我们的结果表明，这些复合物在电子转移之前重新取向。E在水中的溶剂化时间尺度为1皮秒，E的取向弛豫时间为70皮秒。在将E用作DNA电子转移探针时，必须考虑取向和溶剂化效应对E与单核苷酸之间电子转移的影响。
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