Searcharxiv⌕ Search

arXiv subjects

Sophie Marbach

Publications and source records attributed to Sophie Marbach.

31 records · Page 2Linked to original sources

The Nanocaterpillar's Random Walk: Diffusion With Ligand-Receptor Contacts

Particles 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. We demonstrate that the effective diffusion coefficient, which depends on the microscopic parameters governing the legs, can be orders of magnitude smaller than the background diffusion coefficient. Furthermore it varies rapidly with temperature, and reproduces the striking variations seen in existing data and our own measurements of the diffusion of DNA-coated colloids. Our model gives insight into the mechanism of motion, and allows us to ask: when does a nanocaterpillar prefer to move by sliding, where one leg is always linked to the surface, and when does it prefer to move by hopping, which requires all legs to unbind simultaneously? We compare a range of systems (viruses, molecular motors, white blood cells, protein cargos in the nuclear pore complex, bacteria such as Escherichia coli, and DNA-coated colloids) and present guidelines to control the mode of motion for materials design.

cond-mat.soft↗

Comprehensive view of microscopic interactions between DNA-coated colloids

The 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. The range and strength of the interaction are measured and linked to key material design parameters, including DNA sequence, polymer length, grafting density, and complementary fraction. We present a first-principles model that quantitatively reproduces our experimental data without fitting parameters over a wide range of DNA ligand designs. Our theory identifies a subtle competition between DNA binding and steric repulsion and accurately predicts adhesion and melting at a molecular level. Combining experimental and theoretical results, our work provides a quantitative and predictive approach for guiding material design with DNA-nanotechnology and can be further extended to a diversity of colloidal and biological systems.

cond-mat.soft↗

Intrinsic fractional noise in nanopores: The effect of reservoirs

Fluctuations affect nanoporous transport in complex and intricate ways, making optimization of signal-to-noise in artificial designs challenging. Here we focus on the simplest nanopore system, where non-interacting particles diffuse through a pore separating reservoirs. We find that the concentration difference between both sides (akin to the osmotic pressure drop) exhibits fractional noise in time $t$ with mean square average that grows as $t^{1/2}$. This originates from the diffusive exchange of particles from one region to another. We fully rationalize this effect, with particle simulations and analytic solutions. We further infer the parameters (pore radius, pore thickness) that control this exotic behavior. As a consequence, we show that the number of particles within the pore also exhibits fractional noise. Such fractional noise is responsible for noise spectral density scaling as $1/f^{3/2}$ with frequency $f$, and we quantify its amplitude. Our theoretical approach is applicable to more complex nanoporous systems (for example with adsorption within the pore) and drastically simplifies both particle simulations and analytic calculus.

cond-mat.soft↗

Ionic Coulomb blockade as a fractional Wien effect

Recent advances in nanofluidics have allowed 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 tuneable by an external gate -- the ionic analogue of electronic Coulomb blockade (CB) -- would open new avenues in this quest. However, an understanding of ionic CB beyond the electronic analogy is still lacking. Here we show that the many-body dynamics of ions in a charged nanochannel result in a quantised and strongly nonlinear ionic transport, in full agreement with molecular simulations. We find that ionic CB occurs when, upon sufficient confinement, oppositely charged ions form 'Bjerrum pairs', and the conduction proceeds through a mechanism reminiscent of Onsager's Wien effect. Our findings open the way to novel nanofluidic functionalities, such as an ionic-CB-based ion pump inspired by its electronic counterpart.

cond-mat.soft↗

Resonant osmosis across active switchable membranes

To 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. In the presence of an asymmetric membrane, we find a resonant frequency where pumping of solute is performed and can be analyzed in terms of ratchet transport. We discuss and highlight the properties of this resonant osmotic transport. Furthermore, we show that dynamic osmosis allows to pump solute at the nanoscale using less energy than reverse osmosis. This opens new possibilities to build advanced filtration devices and design artificial ionic machinery.

cond-mat.soft↗

Controlling effective dispersion within a channel with flow and active walls

Channels are fundamental building blocks from biophysics to soft robotics, often used to transport or separate solutes. As solute particles inevitably transverse between streamlines along the channel by molecular diffusion, the effective diffusion of the solute along the channel is enhanced - an effect known as Taylor dispersion. Here, we investigate how the Taylor dispersion effect can be suppressed or enhanced in different settings. Specifically, we study the impact of flow profile and active or pulsating channel walls on Taylor dispersion. We derive closed analytic expressions for the effective dispersion equation in all considered scenarios providing hands-on effective dispersion parameters for a multitude of applications. In particular, we find that active channel walls may lead to three regimes of dispersion: either dispersion decrease by entropic slow down at small Peclet number, or dispersion increase at large Peclet number dominated either by shuttle dispersion or by Taylor dispersion. This improves our understanding of solute transport e.g. in biological active systems such as blood flow and opens a number of possibilities to control solute transport in artificial systems such as soft robotics.

cond-mat.soft↗

Local and global force balance for diffusiophoretic transport

Electro- and diffusio- phoresis of particles correspond respectively to the transport of particles under electric field and solute concentration gradients. Such interfacial transport phenomena take their origin in a diffuse layer close to the particle surface, and the motion of the particle is force-free. In the case of electrophoresis, it is further expected that the stress acting on the moving particle vanishes locally as a consequence of local electroneutrality. But the argument does not apply to diffusiophoresis, which takes its origin in solute concentration gradients. In this paper we investigate further the local and global force balance on a particle undergoing diffusiophoresis. We calculate the local tension applied on the particle surface and show that, counter-intuitively, the local force on the particle does not vanish for diffusiophoresis, in spite of the global force being zero as expected. Incidentally, our description allows to clarify the osmotic balance in diffusiophoresis, which has been a source of debates in the recent years. We explore various cases, including hard and soft interactions, as well as porous particles, and provide analytic predictions for the local force balance in these various systems. The existence of local stresses may induce deformation of soft particles undergoing diffusiophoresis, hence suggesting applications in terms of particle separation based on capillary diffusiophoresis.

cond-mat.soft↗

Osmosis, from molecular insights to large-scale applications

Osmosis 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. Here we give a global and unifying view of the phenomenon of osmosis and its consequences with a multi-disciplinary perspective. Pushing the fundamental understanding of osmosis allows to propose new perspectives for different fields and we highlight a number of examples along these lines, for example introducing the concepts of osmotic diodes, active separation and far from equilibrium osmosis, raising in turn fundamental questions in the thermodynamics of separation. The applications of osmosis are also obviously considerable and span very diverse fields. Here we discuss a selection of phenomena and applications where osmosis shows great promises: osmotic phenomena in membrane science (with recent developments in separation, desalination, reverse osmosis for water purification thanks in particular to the emergence of new nanomaterials); applications in biology and health (in particular discussing the kidney filtration process); osmosis and energy harvesting (in particular, osmotic power and blue energy as well as capacitive mixing); applications in detergency and cleaning, as well as for oil recovery in porous media.

cond-mat.soft↗

Active sieving across driven nanopores for tunable selectivity

Molecular separation traditionnally 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. Our analytical and numerical results unveil a rich sieving diagram in terms of the forced gating frequency. Unexpectedly, the separation ability is strongly increased as compared to its passive (zero frequency) counterpart. It points also to the possibility of tuning dynamically the osmotic pressure. Active separation outperforms passive sieving and represents a promising avenue for advanced filtration.

cond-mat.soft↗

Osmotic and diffusio-osmotic flow generation at high solute concentration. I. Mechanical approaches

In 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. We demonstrate in particular how the general expression of the osmotic pressure for mixtures, as obtained classically from the thermodynamic framework, emerges from the mechanical balance controlling non-equilibrium transport under solute gradients. Expressions for the rejection coefficient of osmosis and the diffusio-osmotic mobilities are accordingly obtained. These results generalize existing ones in the dilute solute regime to mixtures with arbitrary concentrations.

cond-mat.soft↗

Osmotic and diffusio-osmotic flow generation at high solute concentration. II. Molecular dynamics simulations

In 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 diffusion-osmotic flow of a solute-solvent fluid adjacent to a solid surface, driven by a chemical potential gradient parallel to the surface. We propose a novel non-equilibrium MD (NEMD) methodology to simulate diffusion-osmosis, by imposing an external force on every particle, which properly mimics the chemical potential gradient on the solute in spite of the periodic boundary conditions. This NEMD method is validated theoretically on the basis of linear-response theory by matching the mobility with their Green-Kubo expressions. Finally, we apply the framework to more realistic systems, namely a water-ethanol mixture in contact with a silica or a graphene surface.

cond-mat.mes-hall↗

Pruning to Increase Taylor Dispersion in Physarum polycephalum Networks

How 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. Pruned networks capitalize on Taylor dispersion to increase the dispersion capability.

physics.bio-ph↗

Active Osmotic Exchanger for Efficient Nanofiltration Inspired by the Kidney

In this paper, we investigate the physical mechanisms underlying one of the most efficient filtration devices: the kidney. Building on a minimal model of the Henle loop - the central part of the kidney filtration - we investigate theoretically the detailed out-of-equilibrium fluxes in this separation process in order to obtain absolute theoretical bounds for its efficiency in terms of separation ability and energy consumption. We demonstrate that this separation process operates at a remarkably small energy cost as compared to traditional sieving processes while working at much smaller pressures. This unique energetic efficiency originates in the double-loop geometry of the nephron, which operates as an active osmotic exchanger. The principles for an artificial-kidney-inspired filtration device could be readily mimicked based on existing soft technologies to build compact and low-energy artificial dialytic devices. Such a "kidney on a chip" also points to new avenues for advanced water recycling, targeting, in particular, sea-water pretreatment for decontamination and hardness reduction.

cond-mat.soft↗