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Charge hopping in DNA.

Y A Berlin1, A L Burin, M A Ratner

  • 1Contribution from the Department of Chemistry, Center for Nanofabrication and Molecular Self-Assembly, and Materials Research Center, Northwestern University, 2145 N Sheridan Road, Evanston, Illinois 60208-3113, USA. berlin@chem.nwu.edu

Journal of the American Chemical Society
|July 18, 2001
PubMed
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Charge migration in DNA is studied, focusing on how holes move through guanine bases. A new model explains how G-base proximity and water reactions affect hole transfer efficiency, crucial for DNA charge transport.

Area of Science:

  • Physical Chemistry
  • Molecular Biophysics
  • Computational Chemistry

Background:

  • Charge migration in DNA is fundamental to its biological functions and potential applications.
  • Understanding hole transfer dynamics is key to explaining DNA's conductivity and reactivity.
  • Existing models often simplify the complex interactions influencing charge transport.

Purpose of the Study:

  • To analyze charge migration efficiency through stacked Watson-Crick base pairs, specifically focusing on guanine (G) bases.
  • To develop a hopping model that accounts for competing processes like hole hopping and reaction with water.
  • To investigate the impact of adjacent guanine units and their vibronic relaxation on hole transfer.

Main Methods:

  • Development of a theoretical hopping model incorporating three competing rate steps: inter-guanine hopping, G(+) reaction with water, and vibronic relaxation within multiple guanine units.

Related Experiment Videos

  • Analysis of the model in two limits: fast charge relaxation within guanine units and slow relaxation.
  • Comparison of model predictions with experimental data for various DNA sequences, including those with GGG triples and GG pairs.

    • Main Results:

    • The model accurately reproduces experimental sequence and distance dependencies for GGG triples in the fast relaxation limit without adjustable parameters.
    • For sequences with adenine:thymine pairs, the model predicts a transition from inverse proportionality to slow exponential decay of hole transfer efficiency with sequence length.
    • Parameters for efficient hole migration through GG pairs were identified by fitting numerical results to experimental data in the slow relaxation limit.

    Conclusions:

    • The proposed hopping model provides a unified framework for understanding charge transfer kinetics in DNA, considering multiple competing processes.
    • The study highlights the critical role of guanine base stacking and surrounding sequences in modulating charge migration efficiency.
    • Further experimental investigations are proposed to refine the understanding of complex charge-transfer hopping mechanisms in DNA.