Effect of structural dynamics on charge transfer in DNA hairpins

Ferdinand C. Grozema, Stefano Tonzani, Yuri A. Berlin, George C Schatz, Laurens D A Siebbeles, Mark A Ratner

Research output: Contribution to journalArticle

122 Citations (Scopus)

Abstract

We present a theoretical study of the positive charge transfer in stilbene-linked DNA hairpins containing only AT base pairs using a tight-binding model that includes a description of structural fluctuations. The parameters are the charge transfer integral between neighboring units and the site energies. Fluctuations in these parameters were studied by a combination of molecular dynamics simulations of the structural dynamics and density functional theory calculations of charge transfer integrals and orbital energies. The fluctuations in both parameters were found to be substantial and to occur on subpicosecond time scales. Tight-binding calculations of the dynamics of charge transfer show that for short DNA hairpins (

Original languageEnglish
Pages (from-to)5157-5166
Number of pages10
JournalJournal of the American Chemical Society
Volume130
Issue number15
DOIs
Publication statusPublished - Apr 16 2008

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Structural dynamics
Charge transfer
DNA
Stilbenes
Molecular Dynamics Simulation
Base Pairing
Theoretical Models
Density functional theory
Molecular dynamics
Computer simulation

ASJC Scopus subject areas

  • Chemistry(all)

Cite this

Effect of structural dynamics on charge transfer in DNA hairpins. / Grozema, Ferdinand C.; Tonzani, Stefano; Berlin, Yuri A.; Schatz, George C; Siebbeles, Laurens D A; Ratner, Mark A.

In: Journal of the American Chemical Society, Vol. 130, No. 15, 16.04.2008, p. 5157-5166.

Research output: Contribution to journalArticle

Grozema, Ferdinand C. ; Tonzani, Stefano ; Berlin, Yuri A. ; Schatz, George C ; Siebbeles, Laurens D A ; Ratner, Mark A. / Effect of structural dynamics on charge transfer in DNA hairpins. In: Journal of the American Chemical Society. 2008 ; Vol. 130, No. 15. pp. 5157-5166.
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