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American Chemical Society, ACS Nano, 9(6), p. 8216-8225, 2012

DOI: 10.1021/nn3030139

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DNA Base Pair Stacks with High Electric Conductance: A Systematic Structural Search

Journal article published in 2012 by Yuri A. Berlin, Alexander A. Voityuk ORCID, Mark A. Ratner
This paper is available in a repository.
This paper is available in a repository.

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Abstract

I nterest in using deoxyribonucleic acid (DNA) as a building block for nanoelec-tronic devices originates from two im-portant properties of this molecule. One property is the ability of DNA to be orga-nized into predictable nanometer-sized structures in both two and three dimen-sions. This remarkable feature has been exploited to obtain a variety of individual constructs including a cube-like molecule, a DNA-truncated octahedron, DNA origami, two-and three-dimensional crystalline ar-rays (for review, see e.g., ref 1) and spherical DNA. 2 The successful assembling of such molecular objects and the subsequent de-sign, formation, and structural evaluation of various unusual DNA motifs clearly demon-strate that DNA has great potential as a "bottom-up" construction material for mak-ing nanoscale templates and machines. 3À5 Another property that makes DNA a promis-ing candidate for a number of applications in molecular electronics is the possibility to con-duct electric current 6À9 transporting charge carriers ("electronic" holes) over distances as large as 40À200 Å. 10À19 This, together with the relative ease to form various constructs, en-ables one to consider DNA as an interesting compound for the design of nanoelectronic circuits. 20,21 For that reason (as well as for the biological relevance), processes of hole trans-fer and transport in DNA have been the sub-jects of extensive research efforts over almost three decades (for comprehensive overview of the field, see e.g., refs 22À25). These efforts have shown that the stacked base pairs inside the double helix provide the pathway for the long-distance charge transport along a DNA molecule, and that the motion of a positive charge primarily generated inside the π-stack array on a particular guanine (G) site could usually be treated as a series of short-range hops between neighboring Gs. 18,26À30 Within this mechanistic picture, each single G is a stepping stone for hole transport, since this base has the lowest oxidation potential among the four native nucleobases. 31À33 Thus, ac-cording to current consensus, the process of hole migration along stacks consisting of gua-nine:cytosine (G:C) base pairs linked by ade-nine:thymine (A:T) bridges is viewed as a series of steps of variable lengths determined by the distance, R, between neighboring Gs (the so-called G-hopping 19). Each elementary step of this multistep motion proceeds via tunneling