Phase behavior and critical activated dynamics of limited-valence DNA nanostars

Silvia Biffi, Roberto Cerbino, Francesca Bomboi, Elvezia Maria Paraboschi, Rosanna Asselta, Francesco Sciortino, Tommaso Bellini

Research output: Contribution to journalArticle

Abstract

Colloidal particles with directional interactions are key in the realization of new colloidal materials with possibly unconventional phase behaviors. Here we exploit DNA self-assembly to produce bulk quantities of DNA stars with three or four sticky terminals, mimicking molecules with controlled limited valence. Solutions of such molecules exhibit a consolution curve with an upper critical point, whose temperature and concentration decrease with the valence. Upon approaching the critical point from high temperature, the intensity of the scattered light diverges with a power law, whereas the intensity time autocorrelation functions show a surprising two-step relaxation, somehow reminiscent of glassy materials. The slow relaxation time exhibits an Arrhenius behavior with no signs of criticality, demonstrating a unique scenario where the critical slowing down of the concentration fluctuations is subordinate to the large lifetime of the DNA bonds, with relevant analogies to critical dynamics in polymer solutions. The combination of equilibrium and dynamic behavior of DNA nanostars demonstrates the potential of DNA molecules in diversifying the pathways toward collective properties and selfassembled materials, beyond the range of phenomena accessible with ordinary molecular fluids.

Original languageEnglish
Pages (from-to)15633-15637
Number of pages5
JournalProceedings of the National Academy of Sciences of the United States of America
Volume110
Issue number39
DOIs
Publication statusPublished - Sep 24 2013

Keywords

  • Critical behavior
  • DNA nanotechnology
  • Limited valence colloids

ASJC Scopus subject areas

  • General

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