Ultrafast Dynamics in DNA-Mediated Electron Transfer: Base Gating and the Role of Temperature

Authors

  • Melanie A. O'Neill,

    1. Laboratory for Molecular Sciences, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology, Pasadena CA, 91 125, USA, Fax: (+1) 626-792-8456
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  • Hans-Christian Becker,

    1. Laboratory for Molecular Sciences, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology, Pasadena CA, 91 125, USA, Fax: (+1) 626-792-8456
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  • Chaozhi Wan,

    1. Laboratory for Molecular Sciences, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology, Pasadena CA, 91 125, USA, Fax: (+1) 626-792-8456
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  • Jacqueline K. Barton,

    1. Laboratory for Molecular Sciences, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology, Pasadena CA, 91 125, USA, Fax: (+1) 626-792-8456
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  • Ahmed H. Zewail

    1. Laboratory for Molecular Sciences, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology, Pasadena CA, 91 125, USA, Fax: (+1) 626-792-8456
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  • This work was made possible through the support of the Laboratory for Molecular Sciences and the NSF. M.A.O. and H.-C.B. are grateful to NSERC and the Wenner-Gren Foundation, respectively, for postdoctoral fellowships.

Abstract

original image

The ultrafast dynamics of electron transfer (ET) between bases in DNA have been determined to elucidate the critical role of base-pair gating on the timescale of the electron transport and the temperature dependence of the rates. ET occurs only through DNA duplexes that adopt a specific, well-coupled alignment of bases (ET-active; see picture). Descriptions of ET dynamics must include fluctuations of DNA bases.

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