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 journalArticle

30 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

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Charge transfer
DNA
Molecular electronics
DNA sequences
Molecular Dynamics Simulation
Absorption spectroscopy
Base Pairing
Ground state
Molecular dynamics
Spectrum Analysis
Geometry
Computer simulation

ASJC Scopus subject areas

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

Cite this

Young, R. M., Singh, A. P. N., K. Thazhathveetil, A., Cho, V. Y., Zhang, Y., Renaud, N., ... Wasielewski, M. R. (2015). Charge transport across DNA-based three-way junctions. Journal of the American Chemical Society, 137(15), 5113-5122. https://doi.org/10.1021/jacs.5b00931

Charge transport across DNA-based three-way junctions. / Young, Ryan M.; Singh, Arunoday P N; K. Thazhathveetil, Arun; Cho, Vincent Y.; Zhang, Yuqi; Renaud, Nicolas; Grozema, Ferdinand C.; Beratan, David N.; Ratner, Mark A; Schatz, George C; Berlin, Yuri A.; Lewis, Frederick D.; Wasielewski, Michael R.

In: Journal of the American Chemical Society, Vol. 137, No. 15, 22.04.2015, p. 5113-5122.

Research output: Contribution to journalArticle

Young, RM, Singh, APN, K. Thazhathveetil, A, Cho, VY, Zhang, Y, Renaud, N, Grozema, FC, Beratan, DN, Ratner, MA, Schatz, GC, Berlin, YA, Lewis, FD & Wasielewski, MR 2015, 'Charge transport across DNA-based three-way junctions', Journal of the American Chemical Society, vol. 137, no. 15, pp. 5113-5122. https://doi.org/10.1021/jacs.5b00931
Young RM, Singh APN, K. Thazhathveetil A, Cho VY, Zhang Y, Renaud N et al. Charge transport across DNA-based three-way junctions. Journal of the American Chemical Society. 2015 Apr 22;137(15):5113-5122. https://doi.org/10.1021/jacs.5b00931
Young, Ryan M. ; Singh, Arunoday P N ; K. Thazhathveetil, Arun ; Cho, Vincent Y. ; Zhang, Yuqi ; Renaud, Nicolas ; Grozema, Ferdinand C. ; Beratan, David N. ; Ratner, Mark A ; Schatz, George C ; Berlin, Yuri A. ; Lewis, Frederick D. ; Wasielewski, Michael R. / Charge transport across DNA-based three-way junctions. In: Journal of the American Chemical Society. 2015 ; Vol. 137, No. 15. pp. 5113-5122.
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