Anion-specific structure and stability of guanidinium-bound DNA origami

Publikation: Beitrag in FachzeitschriftForschungsartikelBeigetragenBegutachtung

Beitragende

  • Marcel Hanke - , Universität Paderborn (Autor:in)
  • Daniel Dornbusch - , Exzellenzcluster PoL: Physik des Lebens, Helmholtz-Zentrum Dresden-Rossendorf (Autor:in)
  • Christoph Hadlich - , Exzellenzcluster PoL: Physik des Lebens, Helmholtz-Zentrum Dresden-Rossendorf (Autor:in)
  • Andre Rossberg - , Helmholtz-Zentrum Dresden-Rossendorf (Autor:in)
  • Niklas Hansen - , Universität Paderborn (Autor:in)
  • Guido Grundmeier - , Universität Paderborn (Autor:in)
  • Satoru Tsushima - , Helmholtz-Zentrum Dresden-Rossendorf (Autor:in)
  • Adrian Keller - , Universität Paderborn (Autor:in)
  • Karim Fahmy - , Helmholtz-Zentrum Dresden-Rossendorf, Technische Universität Dresden (Autor:in)

Abstract

While the folding of DNA into rationally designed DNA origami nanostructures has been studied extensively with the aim of increasing structural diversity and introducing functionality, the fundamental physical and chemical properties of these nanostructures remain largely elusive. Here, we investigate the correlation between atomistic, molecular, nanoscopic, and thermodynamic properties of DNA origami triangles. Using guanidinium (Gdm) as a DNA-stabilizing but potentially also denaturing cation, we explore the dependence of DNA origami stability on the identity of the accompanying anions. The statistical analyses of atomic force microscopy (AFM) images and circular dichroism (CD) spectra reveals that sulfate and chloride exert stabilizing and destabilizing effects, respectively, already below the global melting temperature of the DNA origami triangles. We identify structural transitions during thermal denaturation and show that heat capacity changes ΔCp determine the temperature sensitivity of structural damage. The different hydration shells of the anions and their potential to form Gdm+ ion pairs in concentrated salt solutions modulate ΔCp by altered wetting properties of hydrophobic DNA surface regions as shown by molecular dynamics simulations. The underlying structural changes on the molecular scale become amplified by the large number of structurally coupled DNA segments and thereby find nanoscopic correlations in AFM images.

Details

OriginalspracheEnglisch
Seiten (von - bis)2611-2623
Seitenumfang13
FachzeitschriftComputational and Structural Biotechnology Journal
Jahrgang2022
Ausgabenummer20
PublikationsstatusVeröffentlicht - Jan. 2022
Peer-Review-StatusJa

Schlagworte

Schlagwörter

  • Atomic force microscopy, Circular dichroism, Counteranions, Denaturation, DNA origami, Guanidinium

Bibliotheksschlagworte