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Rae M Robertson-Anderson

Publications and source records attributed to Rae M Robertson-Anderson.

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Starch granules are instructive scaffolds for synergistic reinforcement and dissipation in hydrogel composites

A fundamental challenge in soft material design is the competition between rigidity and dynamicity, as stiffening mechanisms typically suppress energy dissipation. Here, we demonstrate that starch granules serve as instructive scaffolds that overcome this constraint, enabling the synergistic amplification of both elastic reinforcement and dynamic dissipation in hydrogels. We show that engineering the charge and structure of the filler-matrix interface enhances this synergistic response, which we propose arises from a dual-action physical mechanism: filler-induced polymer bundling of the polymer matrix provides structural reinforcement, while transient filler-matrix hydrogen bonding facilitates dissipation. Moreover, we reveal that binary blends of disparate filler species unexpectedly suppress these emergent properties, which we argue arises from enhanced entropic mixing. Our results provide a physical framework to overcome current design limitations in soft composites and sculpt their viscoelastic response from synergistic enhancement to strategic suppression for applications ranging from high-performance soft robotics to biomimetic tissue engineering.

cond-mat.soft

Active and passive crosslinking of cytoskeleton scaffolds tune the effects of cell inclusions on composite structure

Incorporating cells within active biomaterial scaffolds is a promising strategy to develop forefront materials that can autonomously sense, respond, and alter the scaffold in response to environmental cues or internal cell circuitry. Using dynamic biocompatible scaffolds that can self-alter their properties via crosslinking and motor-driven force-generation opens even greater avenues for actuation and control. However, the design principles associated with engineering active scaffolds embedded with cells are not well established. To address this challenge, we design a dynamic scaffold material of bacteria cells embedded within a composite cytoskeletal network of actin and microtubules that can be passively or actively crosslinked by either biotin-streptavidin or multimeric kinesin motors. Using quantitative microscopy, we demonstrate the ability to embed cells of volume fractions 0.4 to 2% throughout the network without compromising the structural integrity of the network or inhibiting crosslinking or motor-driven dynamics. Our findings suggest that both passive and active crosslinking promote entrainment of cells within the network, while depletion interactions play a more important role in uncrosslinked networks. Moreover, we show that large-scale structures emerge with the addition of cell fractions as low as 0.4%, but these structures do not influence the microscale structural lengthscale of the materials. Our work highlights the potential of our composite biomaterial in designing autonomous materials controlled by cells, and provides a roadmap for effectively coupling cells to complex composite materials with an eye towards using cells as in situ factories to program material modifications.

physics.bio-ph

Motor-driven advection competes with crowding to drive spatiotemporally heterogeneous transport in cytoskeleton composites

The cytoskeleton -- a composite network of biopolymers, molecular motors, and associated binding proteins -- is a paradigmatic example of active matter. Particle transport through the cytoskeleton can range from anomalous and heterogeneous subdiffusion to superdiffusion and advection. Yet, recapitulating and understanding these properties -- ubiquitous to the cytoskeleton and other out-of-equilibrium soft matter systems -- remains challenging. Here, we combine light sheet microscopy with differential dynamic microscopy and single-particle tracking to elucidate anomalous and advective transport in actomyosin-microtubule composites. We show that particles exhibit multi-mode transport that transitions from pronounced subdiffusion to superdiffusion at tunable crossover timescales. Surprisingly, while higher actomyosin content enhances superdiffusivity, it also markedly increases the degree of subdiffusion at short timescales and generally slows transport. Corresponding displacement distributions display unique combinations of non-Gaussianity, asymmetry, and non-zero modes, indicative of directed advection coupled with caged diffusion and hopping. At larger spatiotemporal scales, particles undergo superdiffusion which generally increases with actomyosin content, in contrast to normal, yet faster, diffusion without actomyosin. Our specific results shed important new light on the interplay between non-equilibrium processes, crowding and heterogeneity in active cytoskeletal systems. More generally, our approach is broadly applicable to active matter systems to elucidate transport and dynamics across scales.

cond-mat.soft

Ring DNA confers enhanced bulk elasticity and restricted macromolecular diffusion in DNA-dextran blends

Polymer architecture plays critical roles in both bulk rheological properties and microscale macromolecular dynamics in entangled polymer solutions and composites. Ring polymers, in particular, have been the topic of much debate due to the inability of the celebrated reptation model to capture their observed dynamics. Macrorheology and differential dynamic microscopy (DDM) are powerful methods to determine entangled polymer dynamics across scales, yet they typically require different samples under different conditions, preventing direct coupling of bulk rheological properties to the underlying macromolecular dynamics. Here, we perform macrorheology on composites of highly-overlapping DNA and dextran polymers, focusing on the role of DNA topology (rings versus linear chains) as well as the relative volume fractions of DNA and dextran. On the same samples under the same conditions, we perform DDM and single-molecule tracking on embedded fluorescent-labeled DNA molecules immediately before and after bulk measurements. We show DNA-dextran composites exhibit unexpected non-monotonic dependences of bulk viscoelasticity and molecular-level transport properties on the fraction of DNA comprising the composites, with characteristics that are strongly dependent on the DNA topology. We rationalize our results as arising from stretching and bundling of linear DNA versus compaction, swelling, and threading of rings driven by dextran-mediated depletion interactions.

cond-mat.soft

Maximally Stiffening Composites Require Maximally Coupled Rather Than Maximally Entangled Polymer Species

Polymer composites are ideal candidates for next generation biomimetic soft materials because of their exquisite bottom-up designability. However, the richness of behaviours comes at a price: the need for precise and extensive characterisation of material properties over a highly-dimensional parameter space, as well as a quantitative understanding of the physical principles underlying desirable features. Here we couple large-scale Molecular Dynamics simulations with optical tweezers microrheology to characterise the viscoelastic response of DNA-actin composites. We discover that the previously observed non-monotonic stress-stiffening of these composites is robust, yet tunable, in a broad range of the parameter space that spans two orders of magnitude in DNA length. Importantly, we discover that the most pronounced stiffening is achieved when the species are maximally coupled, i.e. have similar number of entanglements, and not when the number of entanglements per DNA chain is largest. We further report novel dynamical oscillations of the microstructure of the composites, alternating between mixed and bundled phases, opening the door to future investigations. The generic nature of our system renders our results applicable to the behaviour of a broad class of polymer composites.

cond-mat.soft