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

doi:10.1021/jacs.5b00931

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

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

39 Scopus citations

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 language	English (US)
Pages (from-to)	5113-5122
Number of pages	10
Journal	Journal of the American Chemical Society
Volume	137
Issue number	15
DOIs	https://doi.org/10.1021/jacs.5b00931
State	Published - Apr 22 2015

ASJC Scopus subject areas

General Chemistry
Biochemistry
Catalysis
Colloid and Surface Chemistry

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10.1021/jacs.5b00931

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title = "Charge transport across DNA-based three-way junctions",

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.",

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

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AU - Young, Ryan M.

AU - Singh, Arunoday P N

AU - K. Thazhathveetil, Arun

AU - Cho, Vincent Y.

AU - Zhang, Yuqi

AU - Renaud, Nicolas

AU - Grozema, Ferdinand C.

AU - Beratan, David N.

AU - Ratner, Mark A.

AU - Schatz, George C.

AU - Berlin, Yuri A.

AU - Lewis, Frederick D.

AU - Wasielewski, Michael R.

PY - 2015/4/22

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AB - 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.

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Charge transport across DNA-based three-way junctions

Abstract

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