Understanding the motion of particles with multivalent ligand-receptors is important for biomedical applications and material design. Yet, even among a single design, the prototypical DNA-coated colloids, seemingly similar micrometric particles hop or roll, depending on the study. We shed light on this problem by observing DNA-coated colloids diffusing near surfaces coated with complementary strands for a wide array of coating designs.
View Article and Find Full Text PDFHypothesis: Through a large parameter space, electric fields can tune colloidal interactions and forces leading to diverse static and dynamical structures. So far, however, field-driven interactions have been limited to dipole-dipole and hydrodynamic contributions. Nonetheless, in this work, we propose that under the right conditions, electric fields can also induce interactions based on local chemical fields and diffusiophoretic flows.
View Article and Find Full Text PDFObserving finite regions of a bigger system is a common aim, from microscopy to molecular simulations. In the latter especially, there is ongoing interest in predicting thermodynamic properties from tracking fluctuations in finite observation volumes. However, kinetic properties have received little attention, especially not in ionic solutions, where electrostatic interactions play a decisive role.
View Article and Find Full Text PDFTransient bonds between fast linkers and slower particles are widespread in physical and biological systems. Despite their diverse structure and function, a commonality is that the linkers diffuse on timescales much faster compared to the overall motion of the particles they bind to. This limits numerical and theoretical approaches that need to resolve these diverse timescales with high accuracy.
View Article and Find Full Text PDFVeins in vascular networks, such as in blood vasculature or leaf networks, continuously reorganize, grow or shrink, to minimize energy dissipation. Flow shear stress on vein walls has been set forth as the local driver for a vein's continuous adaptation. Yet, shear feedback alone cannot account for the observed diversity of vein dynamics - a puzzle made harder by scarce spatiotemporal data.
View Article and Find Full Text PDFInertia does not generally affect the long-time diffusion of passive overdamped particles in fluids. Yet a model starting from the Langevin equation predicts a surprising property of particles coated with ligands that bind reversibly to surface receptors: heavy particles diffuse more slowly than light ones of the same size. We show this by simulation and by deriving an analytic formula for the mass-dependent diffusion coefficient in the overdamped limit.
View Article and Find Full Text PDFCorrection for 'The nanocaterpillar's random walk: diffusion with ligand-receptor contacts' by Sophie Marbach , , 2022, , 3130-3146, DOI: https://doi.org/10.1039/D1SM01544C.
View Article and Find Full Text PDFThe self-assembly of DNA-coated colloids into highly-ordered structures offers great promise for advanced optical materials. However, control of disorder, defects, melting, and crystal growth is hindered by the lack of a microscopic understanding of DNA-mediated colloidal interactions. Here we use total internal reflection microscopy to measure in situ the interaction potential between DNA-coated colloids with nanometer resolution and the macroscopic melting behavior.
View Article and Find Full Text PDFParticles with ligand-receptor contacts bind and unbind fluctuating "legs" to surfaces, whose fluctuations cause the particle to diffuse. Quantifying the diffusion of such "nanoscale caterpillars" is a challenge, since binding events often occur on very short time and length scales. Here we derive an analytical formula, validated by simulations, for the long time translational diffusion coefficient of an overdamped nanocaterpillar, under a range of modeling assumptions.
View Article and Find Full Text PDFTo overcome the traditional paradigm of filtration, where separation is essentially performed upon steric sieving principles, we explore the concept of dynamic osmosis through active membranes. A partially permeable membrane presents a time-tuneable feature that changes the effective pore interaction with the solute and thus actively changes permeability with time. In general, we find that slow flickering frequencies effectively decrease the osmotic pressure and large flickering frequencies do not change it.
View Article and Find Full Text PDFOsmosis is a universal phenomenon occurring in a broad variety of processes and fields. It is the archetype of entropic forces, both trivial in its fundamental expression - the van 't Hoff perfect gas law - and highly subtle in its physical roots. While osmosis is intimately linked with transport across membranes, it also manifests itself as an interfacial transport phenomenon: the so-called diffusio-osmosis and -phoresis, whose consequences are presently actively explored for example for the manipulation of colloidal suspensions or the development of active colloidal swimmers.
View Article and Find Full Text PDFRecent advances in nanofluidics have allowed the exploration of ion transport down to molecular-scale confinement, yet artificial porins are still far from reaching the advanced functionalities of biological ion machinery. Achieving single ion transport that is tunable by an external gate-the ionic analogue of electronic Coulomb blockade-would open new avenues in this quest. However, an understanding of ionic Coulomb blockade beyond the electronic analogy is still lacking.
View Article and Find Full Text PDFMolecular separation traditionally relies on sieving processes across passive nanoporous membranes. Here we explore theoretically the concept of non-equilibrium active sieving. We investigate a simple model for an active noisy nanopore, where gating-in terms of size or charge-is externally driven at a tunable frequency.
View Article and Find Full Text PDFIn this paper, we explore various forms of osmotic transport in the regime of high solute concentration. We consider both the osmosis across membranes and diffusio-osmosis at solid interfaces, driven by solute concentration gradients. We follow a mechanical point of view of osmotic transport, which allows us to gain much insight into the local mechanical balance underlying osmosis.
View Article and Find Full Text PDFIn this paper, we explore osmotic transport by means of molecular dynamics (MD) simulations. We first consider osmosis through a membrane and investigate the reflection coefficient of an imperfectly semi-permeable membrane, in the dilute and high concentration regimes. We then explore the diffusio-osmotic flow of a solute-solvent fluid adjacent to a solid surface, driven by a chemical potential gradient parallel to the surface.
View Article and Find Full Text PDFHow do the topology and geometry of a tubular network affect the spread of particles within fluid flows? We investigate patterns of effective dispersion in the hierarchical, biological transport network formed by Physarum polycephalum. We demonstrate that a change in topology-pruning in the foraging state-causes a large increase in effective dispersion throughout the network. By comparison, changes in the hierarchy of tube radii result in smaller and more localized differences.
View Article and Find Full Text PDFMeasurements and simulations have found that water moves through carbon nanotubes at exceptionally high rates owing to nearly frictionless interfaces. These observations have stimulated interest in nanotube-based membranes for applications including desalination, nano-filtration and energy harvesting, yet the exact mechanisms of water transport inside the nanotubes and at the water-carbon interface continue to be debated because existing theories do not provide a satisfactory explanation for the limited number of experimental results available so far. This lack of experimental results arises because, even though controlled and systematic studies have explored transport through individual nanotubes, none has met the considerable technical challenge of unambiguously measuring the permeability of a single nanotube.
View Article and Find Full Text PDFWe use the theory of active gels to study theoretically the merging and separation of two actin dense layers akin to cortical layers of animal cells. The layers bind at a distance equal to twice the thickness of a free layer, thus forming a single dense layer, similar in this sense to a lamellipodium. When that unique layer is stretched apart, it is resilient to break apart up to a critical length larger than twice the thickness of a free layer.
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