Wirelike charge transport dynamics for DNA-lipid complexes in chloroform

Ashutosh Kumar Mishra, Ryan M. Young, Michael R Wasielewski, Frederick D. Lewis

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

The dynamics of charge separation and charge recombination have been determined for lipid complexes of DNA capped hairpins possessing stilbene electron-acceptor and -donor chromophores separated by base-pair domains that vary in length and base sequence in chloroform solution by means of femtosecond time-resolved transient absorption spectroscopy. The results obtained for the DNA-lipid complexes are compared with those previously obtained in our laboratories for the same hairpins in aqueous buffer. The charge separation and charge recombination times for the lipid complexes are consistently much shorter than those determined in aqueous solution and are only weakly dependent on the number of base pairs separating the acceptor and donor. The enhanced rate constants for forward and return charge transport in DNA-lipid complexes support proposals that solvent gating is responsible, to a significant extent, for the relatively low rates of charge transport for DNA in water. Moreover, they suggest that DNA-lipid complexes may prove useful in the development of DNA-based molecular electronic devices.

Original languageEnglish
Pages (from-to)15792-15797
Number of pages6
JournalJournal of the American Chemical Society
Volume136
Issue number44
DOIs
Publication statusPublished - Nov 5 2014

Fingerprint

Chloroform
Chlorine compounds
Lipids
Charge transfer
DNA
Base Pairing
Genetic Recombination
Molecular electronics
Stilbenes
Chromophores
Absorption spectroscopy
Rate constants
Spectrum Analysis
Buffers
Electrons
Equipment and Supplies
Water

ASJC Scopus subject areas

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

Cite this

Wirelike charge transport dynamics for DNA-lipid complexes in chloroform. / Mishra, Ashutosh Kumar; Young, Ryan M.; Wasielewski, Michael R; Lewis, Frederick D.

In: Journal of the American Chemical Society, Vol. 136, No. 44, 05.11.2014, p. 15792-15797.

Research output: Contribution to journalArticle

Mishra, Ashutosh Kumar ; Young, Ryan M. ; Wasielewski, Michael R ; Lewis, Frederick D. / Wirelike charge transport dynamics for DNA-lipid complexes in chloroform. In: Journal of the American Chemical Society. 2014 ; Vol. 136, No. 44. pp. 15792-15797.
@article{87115be3760b47c78e2230a9e4809ed0,
title = "Wirelike charge transport dynamics for DNA-lipid complexes in chloroform",
abstract = "The dynamics of charge separation and charge recombination have been determined for lipid complexes of DNA capped hairpins possessing stilbene electron-acceptor and -donor chromophores separated by base-pair domains that vary in length and base sequence in chloroform solution by means of femtosecond time-resolved transient absorption spectroscopy. The results obtained for the DNA-lipid complexes are compared with those previously obtained in our laboratories for the same hairpins in aqueous buffer. The charge separation and charge recombination times for the lipid complexes are consistently much shorter than those determined in aqueous solution and are only weakly dependent on the number of base pairs separating the acceptor and donor. The enhanced rate constants for forward and return charge transport in DNA-lipid complexes support proposals that solvent gating is responsible, to a significant extent, for the relatively low rates of charge transport for DNA in water. Moreover, they suggest that DNA-lipid complexes may prove useful in the development of DNA-based molecular electronic devices.",
author = "Mishra, {Ashutosh Kumar} and Young, {Ryan M.} and Wasielewski, {Michael R} and Lewis, {Frederick D.}",
year = "2014",
month = "11",
day = "5",
doi = "10.1021/ja509456q",
language = "English",
volume = "136",
pages = "15792--15797",
journal = "Journal of the American Chemical Society",
issn = "0002-7863",
publisher = "American Chemical Society",
number = "44",

}

TY - JOUR

T1 - Wirelike charge transport dynamics for DNA-lipid complexes in chloroform

AU - Mishra, Ashutosh Kumar

AU - Young, Ryan M.

AU - Wasielewski, Michael R

AU - Lewis, Frederick D.

PY - 2014/11/5

Y1 - 2014/11/5

N2 - The dynamics of charge separation and charge recombination have been determined for lipid complexes of DNA capped hairpins possessing stilbene electron-acceptor and -donor chromophores separated by base-pair domains that vary in length and base sequence in chloroform solution by means of femtosecond time-resolved transient absorption spectroscopy. The results obtained for the DNA-lipid complexes are compared with those previously obtained in our laboratories for the same hairpins in aqueous buffer. The charge separation and charge recombination times for the lipid complexes are consistently much shorter than those determined in aqueous solution and are only weakly dependent on the number of base pairs separating the acceptor and donor. The enhanced rate constants for forward and return charge transport in DNA-lipid complexes support proposals that solvent gating is responsible, to a significant extent, for the relatively low rates of charge transport for DNA in water. Moreover, they suggest that DNA-lipid complexes may prove useful in the development of DNA-based molecular electronic devices.

AB - The dynamics of charge separation and charge recombination have been determined for lipid complexes of DNA capped hairpins possessing stilbene electron-acceptor and -donor chromophores separated by base-pair domains that vary in length and base sequence in chloroform solution by means of femtosecond time-resolved transient absorption spectroscopy. The results obtained for the DNA-lipid complexes are compared with those previously obtained in our laboratories for the same hairpins in aqueous buffer. The charge separation and charge recombination times for the lipid complexes are consistently much shorter than those determined in aqueous solution and are only weakly dependent on the number of base pairs separating the acceptor and donor. The enhanced rate constants for forward and return charge transport in DNA-lipid complexes support proposals that solvent gating is responsible, to a significant extent, for the relatively low rates of charge transport for DNA in water. Moreover, they suggest that DNA-lipid complexes may prove useful in the development of DNA-based molecular electronic devices.

UR - http://www.scopus.com/inward/record.url?scp=84908691499&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84908691499&partnerID=8YFLogxK

U2 - 10.1021/ja509456q

DO - 10.1021/ja509456q

M3 - Article

C2 - 25299823

AN - SCOPUS:84908691499

VL - 136

SP - 15792

EP - 15797

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 44

ER -