Mechanical response of a simple DNA nanostar hydrogel: symptoms of disorder and glassy emergence of solidity

Abstract: DNA self-assembly is a well-understood nanotechnology to obtain extremely ordered structures from the nanometer to up to the hundred of microns scale. By contrast, DNA hydrogels rely on the disordered assembly of DNA building blocks to reach macroscopic volumes. However, in order to hold the promise of DNA bulk materials, the sequence designer needs a systematic understanding of how macroscopic properties emerge from disorder. Here, we show a method to study systematically the mechanical response of a simple DNA nanostar hydrogel. This method mobilises bulk rheology, dynamic light scattering microrheology, mechanical modeling, as well as thermodynamic calculation and DNA sequence alteration. At low temperatures, we demonstrate a systematic deviation from Maxwell behaviour that is symptomatic of disordered materials. At temperatures much higher than the percolation of the DNA network, we characterise a surprising solid behaviour that we attribute to a glass transition. Our results show the importance of disorder in DNA materials. Furthermore, the method we showcase in this article can be widely applied to more complex DNA materials.