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Articles linked to this work by shared authors, journal, and citation graph.

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Tracking Photoinduced Charge Separation in DNA: from Start to Finish.

Accounts of chemical research·2018
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Fluorescent excimers and exciplexes of the purine base derivative 8-phenylethynyl-guanine in DNA hairpins.

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Tracking Hole Transport in DNA Hairpins Using a Phenylethynylguanine Nucleobase.

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Structure and Dynamics of Electron Injection and Charge Recombination in i-Motif DNA Conjugates.

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Dynamics of Charge Injection and Charge Recombination in DNA Mini-Hairpins.

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Self-Assembly of Perylenediimide-Single-Strand-DNA Conjugates: Employing Hydrophobic Interactions and DNA Base-Pairing To Create a Diverse Structural Space.

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DNA electron transfer mechanism and dynamics.

Frederick D Lewis1

  • 1Department of Chemistry, Northwestern University, Evanston, Illinois, USA. fdl@northwestern.edu

Nucleic Acids Symposium Series (2004)
|September 9, 2008
PubMed
Summary

Photoinduced charge separation in DNA hairpins depends on linker distance. Short distances use superexchange, while longer distances involve multistep hole transport influenced by sequence and a Coulomb cage effect.

Area of Science:

  • Molecular Biophysics
  • Photochemistry
  • Synthetic Biology

Background:

  • Investigating photoinduced charge separation in synthetic DNA structures is crucial for understanding energy transfer mechanisms.
  • Stilbene-based linkers (stilbenedicarboxamide and stilbene-diether) are employed to study charge transport dynamics.

Purpose of the Study:

  • To elucidate the mechanisms and efficiency of photoinduced charge separation in DNA hairpins and dumbbells.
  • To determine the influence of linker separation distance and DNA sequence on charge transport dynamics.

Main Methods:

  • Time-resolved fluorescence spectroscopy
  • Transient absorption spectroscopy
  • Investigation of synthetic DNA hairpins and dumbbells with varying linker separations and base pair sequences.

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Main Results:

  • Charge separation proceeds via superexchange at short distances and multistep hole transport at longer distances (≥2 base pairs).
  • Hole transport efficiency is highly distance-dependent for short separations, attributed to a Coulomb cage effect, and less sensitive at larger distances.
  • Hole transport is less efficient across alternating AT sequences compared to poly(dA) sequences. Guanine incorporation impacts charge separation efficiency based on its location.

Conclusions:

  • The mechanism and efficiency of charge separation in synthetic DNA are modulated by linker separation, DNA sequence, and environmental effects like the Coulomb cage.
  • Understanding these dynamics provides insights into designing DNA-based molecular wires and electronic devices.