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

33 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

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

Access to Document

10.1021/jacs.5b00931

Fingerprint Dive into the research topics of 'Charge transport across DNA-based three-way junctions'. Together they form a unique fingerprint.

Cite this

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.

@article{aa2bb63c612c48a0925f1e97e58fa302,

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.}",

year = "2015",

month = apr,

day = "22",

doi = "10.1021/jacs.5b00931",

language = "English (US)",

volume = "137",

pages = "5113--5122",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "15",

}

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 journal › Article › peer-review

TY - JOUR

T1 - Charge transport across DNA-based three-way junctions

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

Y1 - 2015/4/22

N2 - 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.

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.

UR - http://www.scopus.com/inward/record.url?scp=84928501352&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84928501352&partnerID=8YFLogxK

U2 - 10.1021/jacs.5b00931

DO - 10.1021/jacs.5b00931

M3 - Article

C2 - 25822073

AN - SCOPUS:84928501352

VL - 137

SP - 5113

EP - 5122

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 15

ER -