SignificanceWhile widely known as the molecule of life, DNA is also an amazing building block at the nanoscale, since it allows us to design and program the structure and dynamics of functional nanomaterials. We exploit the programmability of DNA to achieve control over the rheology of self-assembled hydrogels, which have elastic or viscous behavior (similar to that of slime) that is finely regulated by temperature. Using microrheology to investigate the mechanical properties of DNA hydrogels at the microlength scale, we map the viscoelastic response over a broad range of frequencies and temperatures. The deep understanding in the fundamental physics provides a way to design DNA-based materials with precise control over the structure stability and rigidity at molecular level.
We present thermophoretic measurements in aqueous suspensions of three different polystyrene (PS) particles of varying negative charge, size, and surface coating. Our measurement technique is based on the observation of the colloidal steady-state distribution using conventional bright-field microscopy, which avoids undesirable effects such as laser-induced convection or local heating. We find that the colloids with the weakest zeta potential exhibit the strongest thermophoretic effect, suggesting that the Soret coefficient has a more intricate dependence on surface functionality than predicted by existing theoretical approaches. We also study the relaxation of the colloids to steady-state and propose a model to quantify the relaxation speed, based on the time evolution of the colloidal center of mass. Our observations are well described by this model and show that the relaxation speed tends to increase with the magnitude of the thermophoretic force.
Fluorinated latex particles were synthesized and functionalized with single stranded-DNA, facilitating controlled aggregation into porous gel networks; these can be studied deep into the bulk phase due to refractive-index matching.
DNA has emerged as an exciting binding agent for programmable colloidal self-assembly. Its popularity derives from its unique properties: it provides highly specific short-ranged interactions and at the same time it acts as a steric stabilizer against non-specific van der Waals and Coulomb interactions. Because complementary DNA strands are linked only via hydrogen bonds, DNA-mediated binding is thermally reversible: it provides an effective attraction that can be switched off by raising the temperature only by a few degrees. In this article we introduce a new binary system made of DNA-functionalized filamentous fd viruses of ∼880 nm length with an aspect ratio of ∼100, and 50 nm gold nanoparticles (gold NPs) coated with the complementary DNA strands. When quenching mixtures below the melt temperature Tm, at which the attraction is switched on, we observe aggregation. Conversely, above Tm the system melts into a homogenous particulate 'gas'. We present the aggregation behavior of three different gold NP to virus ratios and compare them to a gel made solely of gold NPs. In particular, we have investigated the aggregate structures as a function of cooling rate and determine how they evolve as function of time for given quench depths, employing fluorescence microscopy. Structural information was extracted in the form of an effective structure factor and chord length distributions. Rapid cooling rates lead to open aggregates, while slower controlled cooling rates closer to equilibrium DNA hybridization lead to more fine-stranded gels. Despite the different structures we find that for both cooling rates the quench into the two-phase region leads to initial spinodal decomposition, which becomes arrested. Surprisingly, although the fine-stranded gel is disordered, the overall structure and the corresponding length scale distributions in the system are remarkably reproducible. Such highly porous systems can be developed into new functional materials.
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