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Self-Assembly of All-DNA Rods with Controlled Patchiness.

Katarina Gvozden1, Sanja Novak Ratajczak1, Alberto G Orellana2

  • 1Biomacromolecular Systems and Processes, Institute of Biological Information Processing (IBI-4), Forschungszentrum Jülich, D-52425, Jülich, Germany.

Small (Weinheim an Der Bergstrasse, Germany)
|November 27, 2021
PubMed
Summary

Stiff double-stranded DNA (dsDNA) fragments self-assemble into liquid crystal phases by controlling blunt-end attractions. This study engineers DNA interactions to stabilize elusive smectic-A phases, opening new avenues for DNA-based materials.

Keywords:
DNAliquid crystalspatchy particlesself-assembly

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Area of Science:

  • Biophysics
  • Materials Science
  • Supramolecular Chemistry

Background:

  • Double-stranded DNA (dsDNA) fragments possess inherent noncovalent attractive interactions at their tips.
  • The influence of these blunt-end attractions on DNA liquid crystal self-assembly remains poorly understood.

Purpose of the Study:

  • To investigate how selective screening of blunt-end DNA stacking interactions affects the self-assembly of dsDNA fragments into liquid crystalline phases.
  • To engineer DNA duplexes to control blunt-end attractions and stabilize novel DNA-based liquid crystal phases.

Main Methods:

  • Constructing DNA duplexes with short hairpin caps to selectively screen blunt-end attractions.
  • Utilizing concentrated aqueous solutions to induce self-assembly of engineered dsDNA fragments.
  • Employing Monte-Carlo simulations of hard cylinders with attractive terminal sites to confirm phase existence.

Main Results:

  • Stiff dsDNA fragments with moderate aspect ratios self-assemble into various smectic mesophases by modulating blunt-end attractions.
  • Engineered DNA duplexes stabilized all-DNA bilayer and monolayer smectic-A phases, as well as a columnar phase.
  • The study confirmed the thermodynamic stability of the smectic-A phase in rod-like DNA liquid crystals and the existence of the bilayer smectic phase.

Conclusions:

  • DNA blunt-ends function as tunable monovalent attractive patches.
  • Precise control over DNA blunt-end interactions enables the stabilization of nonconventional DNA-based lyotropic liquid crystal phases.
  • This work presents unique opportunities for designing arbitrary geometry and composition DNA-based patchy particles for advanced materials.