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Excited States in Single-Stranded and i-Motif DNA with Silver Ions.

Zakhar V Reveguk1, Evgeny V Khoroshilov2, Andrey V Sharkov2

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Silver ions bind to cytosine DNA chains, forming duplexes stabilized by C-Ag+-C bonds. This binding alters DNA structure and excited-state properties, depending on ion concentration and binding sites.

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Area of Science:

  • Biophysical Chemistry
  • Molecular Biophysics
  • DNA Nanotechnology

Background:

  • Cytosine-rich DNA sequences can form complex structures like i-motifs.
  • Silver ions (Ag+) are known to interact with DNA, influencing its structure and properties.
  • Understanding these interactions is crucial for developing novel DNA-based materials and therapeutics.

Purpose of the Study:

  • To investigate the structural and excited-state properties of cytosine (dC)10 chains complexed with silver ions (Ag+).
  • To determine the effect of varying Ag+ concentrations and pH on DNA complex formation and stability.
  • To elucidate the binding sites and mechanisms of Ag+ interaction with cytosine.

Main Methods:

  • Circular dichroism (CD) spectroscopy.
  • Steady-state absorption and fluorescence spectroscopy.
  • Ultrafast fluorescence upconversion spectroscopy.
  • Computational calculation of vertical electronic transition energies.

Main Results:

  • (dC)10 chains form Ag+-stabilized duplexes via C-Ag+-C bonds.
  • The i-motif structure of (dC)10 is destabilized by the presence of Ag+ ions.
  • Excited-state properties are modulated by Ag+ binding, with new low-lying states appearing upon interaction with cytosine's O or N7 atoms.

Conclusions:

  • Silver ions induce significant structural changes in cytosine-rich DNA, favoring duplex formation over i-motif structures.
  • The binding site and stoichiometry of Ag+ ions dictate the observed changes in excited-state dynamics.
  • These findings provide insights into metal-DNA interactions with implications for DNA nanotechnology and sensing applications.