Charge transport across DNA-based three-way junctions

Ryan M. Young, Arunoday P.N. Singh, Arun K. Thazhathveetil, Vincent Y. Cho, Yuqi Zhang, Nicolas Renaud, Ferdinand C. Grozema, David N. Beratan, Mark A. Ratner, George C. Schatz, Yuri A. Berlin, Frederick D. Lewis, Michael R. Wasielewski

Research output: Contribution to journalArticlepeer-review

32 Citations (Scopus)

Abstract

DNA-based molecular electronics will require charges to be transported from one site within a 2D or 3D architecture to another. While this has been shown previously in linear, π-stacked DNA sequences, the dynamics and efficiency of charge transport across DNA three-way junction (3WJ) have yet to be determined. Here, we present an investigation of hole transport and trapping across a DNA-based three-way junction systems by a combination of femtosecond transient absorption spectroscopy and molecular dynamics simulations. Hole transport across the junction is proposed to be gated by conformational fluctuations in the ground state which bring the transiently populated hole carrier nucleobases into better aligned geometries on the nanosecond time scale, thus modulating the π-π electronic coupling along the base pair sequence.

Original languageEnglish
Pages (from-to)5113-5122
Number of pages10
JournalJournal of the American Chemical Society
Volume137
Issue number15
DOIs
Publication statusPublished - Apr 22 2015

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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