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Excess Electron Transfer through DNA Duplexes Comprising a Metal-Mediated Base Pair.

Susanne Hensel1, Kevin Eckey1, Philipp Scharf1

  • 1Westfälische Wilhelms-Universität Münster, Institut für Anorganische und Analytische Chemie, Corrensstraße 30, 48149, Münster, Germany.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|June 29, 2017
PubMed
Summary

Metal-mediated thymine-HgII-thymine base pairs in DNA duplexes hinder excess electron transfer. Even one such pair significantly reduces charge transfer efficiency, while two contiguous pairs effectively block it.

Keywords:
DNAcharge transfermercurymetal-mediated base pairthymine

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Area of Science:

  • Bioorganic Chemistry
  • Supramolecular Chemistry
  • Molecular Biophysics

Background:

  • Investigating charge transfer through DNA is crucial for developing molecular electronics and understanding DNA repair mechanisms.
  • Metal-mediated base pairs offer unique structural and electronic properties for modulating DNA conductivity.
  • Thymine-mercury(II)-thymine base pairs represent a specific modification for studying electron transfer pathways.

Purpose of the Study:

  • To quantify the efficiency of excess electron transfer across DNA duplexes containing one or two thymine-HgII-thymine metal-mediated base pairs.
  • To compare the charge transfer efficiency through these metal-mediated base pairs with canonical base pairs and thymine-thymine mispairs.
  • To assess the impact of contiguous metal-mediated base pairs on electron transfer dynamics.

Main Methods:

  • Synthesis of DNA duplexes incorporating an artificial electron donor (dN) and an electron acceptor (dB).
  • Introduction of one or two thymine-HgII-thymine metal-mediated base pairs within the DNA duplex.
  • Quantification of charge transfer efficiency using Liquid Chromatography with Inductively Coupled Plasma Mass Spectrometry (LC/ICP-MS) to measure unreacted electron acceptor after photo-irradiation.
  • Utilizing canonical adenine:thymine base pairs as a reference for charge transfer detection.

Main Results:

  • Excess electron transfer across a single thymine-HgII-thymine base pair exhibits low efficiency, similar to a thymine:thymine mispair.
  • The presence of two contiguous thymine-HgII-thymine base pairs effectively inhibits excess electron transfer through the DNA duplex.
  • The methodology using LC/ICP-MS is validated for detecting charge transfer in DNA by comparison with canonical base pairs.

Conclusions:

  • Thymine-HgII-thymine metal-mediated base pairs act as significant barriers to excess electron transfer in DNA duplexes.
  • The efficiency of charge transfer is highly sensitive to the number and arrangement of metal-mediated base pairs.
  • These findings provide insights into the design of DNA-based electronic components and the fundamental mechanisms of charge transport in modified nucleic acids.