Time dependence of advection-diffusion coupling for nanoparticle ensembles

Advection-diffusion coupling can enhance particle and solute dispersion by orders of magnitude as compared to pure diffusion, with a steady state being reached for confined flow regions such as a nanopore or blood vessel. Here, by using evanescent wave microscopy, we measure for the first time the full dynamics of Taylor dispersion, highlighting the crucial role of the initial concentration profile. We make time-dependent, nanometrically resolved particle dispersion measurements varying nanoparticle size, velocity gradient, and viscosity in submicrometric near-surface flows. Such resolution permits a measure of the full dynamical approach and crossover into the steady state, revealing a family of master curves. Remarkably, our results show that the dynamics depend sensitively on the initial spatial distribution of the nanoparticles. These observations are in quantitative agreement with existing analytical models and numerical simulations performed herein. We anticipate that our study will be a first step toward observing and modelling more complex situations at the nanoscale, such as target finding and chemical reactions in nanoconfined flows, dynamical adsorption and capture problems, as well as nanoscale drug delivery systems.

Automated summary

In this study, advection-diffusion coupling is found to greatly enhance particle and solute dispersion compared to pure diffusion, with the dynamics being sensitive to the initial spatial distribution of nanoparticles. The measurements conducted using evanescent wave microscopy reveal a family of master curves, showing the crucial role of initial concentration profiles. These findings are in quantitative agreement with existing analytical models and numerical simulations.