RESUMO
Understanding and controlling the rheology of polymeric complex fluids that are pushed out-of-equilibrium is a fundamental problem in both industry and biology. For example, to package, repair, and replicate DNA, cells use enzymes to constantly manipulate DNA topology, length, and structure. Inspired by this feat, here we engineer and study DNA-based complex fluids that undergo enzymatically-driven topological and architectural alterations via restriction endonuclease (RE) reactions. We show that these systems display time-dependent rheological properties that depend on the concentrations and properties of the comprising DNA and REs. Through time-resolved microrheology experiments and Brownian Dynamics simulations, we show that conversion of supercoiled to linear DNA topology leads to a monotonic increase in viscosity. On the other hand, the viscosity of entangled linear DNA undergoing fragmentation displays a universal decrease that we rationalise using living polymer theory. Finally, to showcase the tunability of these behaviours, we design a DNA fluid that exhibits a time-dependent increase, followed by a temporally-gated decrease, of its viscosity. Our results present a class of polymeric fluids that leverage naturally occurring enzymes to drive diverse time-varying rheology by performing architectural alterations to the constituents.
Assuntos
DNA , Polímeros , Digestão , Reologia , ViscosidadeRESUMO
Anomalous diffusion in crowded and complex environments is widely studied due to its importance in intracellular transport, fluid rheology and materials engineering. Specifically, diffusion through the cytoskeleton, a network comprised of semiflexible actin filaments and rigid microtubules that interact both sterically and via crosslinking, plays a principal role in viral infection, vesicle transport and targeted drug delivery. Here, we elucidate the impact of crosslinking on particle diffusion in composites of actin and microtubules with actin-actin, microtubule-microtubule and actin-microtubule crosslinking. We analyze a suite of transport metrics by coupling single-particle tracking and differential dynamic microscopy. Using these complementary techniques, we find that particles display non-Gaussian and non-ergodic subdiffusion that is markedly enhanced by cytoskeletal crosslinking, which we attribute to suppressed microtubule mobility. However, the extent to which transport deviates from normal Brownian diffusion depends strongly on the crosslinking motif - with actin-microtubule crosslinking inducing the most pronounced anomalous characteristics. Our results reveal that subtle changes to actin-microtubule interactions can have complex impacts on particle diffusion in cytoskeleton composites, and suggest that a combination of reduced filament mobility and more variance in actin mobilities leads to more strongly anomalous particle transport.
Assuntos
Actinas , Microtúbulos , Citoesqueleto de Actina , Citoesqueleto , DifusãoRESUMO
[This corrects the article DOI: 10.1371/journal.pone.0176732.].
RESUMO
We characterize the lengthscale-dependent rheological properties of mucus from the ubiquitous Chaetopterus marine worm. We use optically trapped probes (2-10 µm) to induce microscopic strains and measure the stress response as a function of oscillation amplitude. Our results show that viscoelastic properties are highly dependent on strain scale (l), indicating three distinct lengthscale-dependent regimes at l1 ≤4 µm, l2≈4-10 µm, and l3≥10 µm. While mucus response is similar to water for l1, suggesting that probes rarely contact the mucus mesh, the response for l2 is distinctly more viscous and independent of probe size, indicative of continuum mechanics. Only for l3 does the response match the macroscopic elasticity, likely due to additional stiffer constraints that strongly resist probe displacement. Our results suggest that, rather than a single lengthscale governing crossover from viscous to elastic, mucus responds as a hierarchical network with a loose biopolymer mesh coupled to a larger scaffold responsible for macroscopic gel-like mechanics.
