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Charge splitters and charge transport junctions based on guanine quadruplexes

Abstract

Self-assembling circuit elements, such as current splitters or combiners at the molecular scale, require the design of building blocks with three or more terminals. A promising material for such building blocks is DNA, wherein multiple strands can self-assemble into multi-ended junctions, and nucleobase stacks can transport charge over long distances. However, nucleobase stacking is often disrupted at junction points, hindering electric charge transport between the two terminals of the junction. Here, we show that a guanine-quadruplex (G4) motif can be used as a connector element for a multi-ended DNA junction. By attaching specific terminal groups to the motif, we demonstrate that charges can enter the structure from one terminal at one end of a three-way G4 motif, and can exit from one of two terminals at the other end with minimal carrier transport attenuation. Moreover, we study four-way G4 junction structures by performing theoretical calculations to assist in the design and optimization of these connectors.

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Fig. 1: Structures and conductance measurements for G4+3 constructs.
Fig. 2: Measured conductance, molecular dynamics simulations and electronic coupling strength calculations for antiparallel and parallel G4+3 junctions.
Fig. 3: Structures, conductance, molecular dynamics simulations, and electronic coupling strength calculations for antiparallel and parallel G4+4 constructs.

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Acknowledgements

We thank the Office of Naval Research (N00014-11-1-0729) for support.

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Contributions

R.S. and N.C.S. designed and synthesized the DNA molecules. L.X., Y.L. and N.T. designed and conducted the conductance measurements experiments. C.L., A.B., Y.Z., P.Z. and D.N.B. conducted and analysed the simulations. The three teams collaborated intensively in formulating the key molecular designs, analysing the data and writing the manuscript.

Corresponding authors

Correspondence to David N. Beratan or Nongjian Tao or Nadrian C. Seeman.

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The authors declare no competing interests.

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Supplementary Figures 1–11, Supplementary Tables 1–2, Supplementary Notes 1–3.

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Sha, R., Xiang, L., Liu, C. et al. Charge splitters and charge transport junctions based on guanine quadruplexes. Nature Nanotech 13, 316–321 (2018). https://doi.org/10.1038/s41565-018-0070-x

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