Current Fluctuations in Nanopores Reveal the Polymer-Wall Adsorption Potential.

Modification of surface properties by polymer adsorption is a widely used technique to tune interactions in molecular experiments such as nanopore sensing. Here, we investigate how the ionic current noise through solid-state nanopores reflects the adsorption of short, neutral polymers to the pore surface. The power spectral density of the noise shows a characteristic change upon adsorption of polymer, the magnitude of which is strongly dependent on both polymer length and salt concentration. In particular, for short polymers at low salt concentrations no change is observed, despite the verification of comparable adsorption in these systems using quartz crystal microbalance measurements. We propose that the characteristic noise is generated by the movement of polymers on and off the surface and perform simulations to assess the feasibility of this model. Excellent agreement with experimental data is obtained using physically motivated simulation parameters, providing deep insight into the shape of the adsorption potential and underlying processes. This paves the way toward using noise spectral analysis for in situ characterization of functionalized nanopores.

Observing capture with a colloidal model membrane channel.

We use video microscopy to study the full capture process for colloidal particles transported through microfluidic channels by a pressure-driven flow. In particular, we obtain trajectories for particles as they move from the bulk into confinement, using these to map in detail the spatial velocity and concentration fields for a range of different flow velocities. Importantly, by changing the height profiles of our microfluidic devices, we consider systems for which flow profiles in the channel are the same, but flow fields in the reservoir differ with respect to the quasi-2D monolayer of particles. We find that velocity fields and profiles show qualitative agreement with numerical computations of pressure-driven fluid flow through the systems in the absence of particles, implying that in the regimes studied here particle-particle interactions do not strongly perturb the flow. Analysis of the particle flux through the channel indicates that changing the reservoir geometry leads to a change between long-range attraction of the particles to the pore and diffusion-to-capture-like behaviour, with concentration fields that show qualitative changes based on device geometry. Our results not only provide insight into design considerations for microfluidic devices, but also a foundation for experimental elucidation of the concept of a capture radius. This long standing problem plays a key role in transport models for biological channels and nanopore sensors.