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 language | English |
|---|---|
| Pages (from-to) | 15792-15797 |
| Number of pages | 6 |
| Journal | Journal of the American Chemical Society |
| Volume | 136 |
| Issue number | 44 |
| DOIs | |
| Publication status | Published - Nov 5 2014 |
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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 journal › Article
}
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 -