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Intermediate tunnelling–hopping regime in DNA charge transport

Nature Chemistry volume 7, pages 221226 (2015) | Download Citation

  • A Corrigendum to this article was published on 21 February 2017

This article has been updated

Abstract

Charge transport in molecular systems, including DNA, is involved in many basic chemical and biological processes, and its understanding is critical if they are to be used in electronic devices. This important phenomenon is often described as either coherent tunnelling over a short distance or incoherent hopping over a long distance. Here, we show evidence of an intermediate regime where coherent and incoherent processes coexist in double-stranded DNA. We measure charge transport in single DNA molecules bridged to two electrodes as a function of DNA sequence and length. In general, the resistance of DNA increases linearly with length, as expected for incoherent hopping. However, for DNA sequences with stacked guanine–cytosine (GC) base pairs, a periodic oscillation is superimposed on the linear length dependence, indicating partial coherent transport. This result is supported by the finding of strong delocalization of the highest occupied molecular orbitals of GC by theoretical simulation and by modelling based on the Büttiker theory of partial coherent charge transport.

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Change history

  • 17 January 2017

    In the version of this Article originally published, in ref. 19, in the author list, the second, third and fourth authors were not included and the reference should have read: 'Grib, N. V., Ryndyk, D. A., Gutiérrez, R. & Cuniberti, G. Distance-dependent coherent charge transport in DNA: crossover from tunneling to free propagation. J. Biophys. Chem. 1, 77–85 (2010).' This has now been corrected in the online versions of this Article.

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Acknowledgements

The authors thank S. Jiang and H. Yan for help with PAGE gel experiments, and D.N. Beratan, N. Seeman, F.D. Lewis, Y. Berlin, A. Balaeff and M.R. Wasielewski for discussions. The authors also acknowledge financial support from the Office of Naval Research (N00014-11-1-0729).

Author information

Affiliations

  1. Center for Biosensors and Bioelectronics, Biodesign Institute, Arizona State University, Tempe, Arizona 85287, USA

    • Limin Xiang
    • , Julio L. Palma
    • , Christopher Bruot
    •  & Nongjian Tao
  2. Department of Chemistry and Biochemistry, Arizona State University, Tempe, Arizona 85287, USA

    • Limin Xiang
    • , Julio L. Palma
    •  & Vladimiro Mujica
  3. Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA

    • Mark A. Ratner
  4. School of Electrical, Computer and Energy Engineering, Arizona State University, Tempe, Arizona 85287, USA

    • Nongjian Tao

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Contributions

L.X. and C.B. performed the conductance measurement experiments. J.L.P. performed INDO calculations. M.A.R. and V.M. supervised the INDO calculations. N.T. proposed the Büttiker model analysis and supervised the experiments.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Nongjian Tao.

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DOI

https://doi.org/10.1038/nchem.2183

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