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Duplex polarons in DNA.

Esther M Conwell1, Steven M Bloch, Patrick M McLaughlin

  • 1Department of Chemistry, University of Rochester, Rochester, New York 14627, USA. conwell@chem.rochester.edu

Journal of the American Chemical Society
|June 26, 2007
PubMed
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This study models solvated polarons in DNA, finding that charge distribution on two complementary base chains increases binding energy. The polaron wavefunction primarily localizes on the initially charged chain, contradicting zigzag hole transport theories.

Area of Science:

  • Computational Chemistry
  • Molecular Biophysics
  • DNA Charge Transport

Background:

  • Previous models simplified solvated polarons in DNA by localizing charge on a single base chain.
  • Understanding charge distribution is crucial for elucidating charge transport mechanisms in DNA.

Purpose of the Study:

  • To investigate the behavior of solvated polarons in DNA when charge is distributed across two complementary base chains.
  • To determine the effect of this charge distribution on polaron binding energy and wavefunction localization.
  • To compare computational findings with experimental results and challenge existing theories of DNA charge transport.

Main Methods:

  • Extended theoretical calculations to model charge distributed on two complementary DNA base chains.
  • Calculated polaron wavefunction and binding energy for various DNA sequences.

Related Experiment Videos

  • Analyzed polaron localization and compared results with experimental data.

    • Main Results:

    • Distributing charge on two complementary chains increases polaron binding energy compared to single-chain models.
    • The polaron wavefunction predominantly localizes on the chain initially holding the charge.
    • This localization occurs even when lower energy sites are available on the complementary chain.

    Conclusions:

    • The study provides a more realistic model for solvated polarons in DNA by considering charge distribution.
    • Findings support experimental observations and contradict theories suggesting zigzag hole transport between DNA strands.
    • The predominant localization of the polaron wavefunction has significant implications for understanding charge mobility in DNA.