Dynamics and ordering of weakly Brownian particles in directional drying

TL;DR

This study investigates how particle velocity influences the ordering of weakly Brownian particles during directional drying, revealing that faster flow leads to denser packing and higher ordering, contrasting with Brownian particles.

Contribution

It provides the first direct measurement of particle velocities and their correlation with ordering during drying, highlighting the role of flow velocity in particle packing.

Findings

Higher particle velocities lead to increased ordering.

Faster flow causes denser particle packing.

Behavior differs from Brownian particles, which reorganize via Brownian motion.

Abstract

Drying of particle suspensions is an ubiquitous phenomenon with many natural and practical applications. In particular, in unidirectional drying, the evaporation of the solvent induces flows which accumulate particles at the liquid/air interface. The progressive build-up of a dense region of particles can be used, in particular, in the processing of advanced materials and architectures while the development of heterogeneities and defects in such systems is critical to their function. A lot of attention has thus been paid to correlate the flow and particles dynamics to the ordering of particles. However, dynamic observation at the particle scale and its correlation with local particle ordering are still missing. Here we show by measuring the particle velocities with high frame rate laser scanning confocal microscopy that the ordering of weakly Brownian particles during directional drying in a Hele-Shaw cell opened on one side depends on the particle velocity. Under the ambient and experimental conditions presented in the following, the particle velocities accumulate in two branches. A higher degree of ordering is found for the branch of faster particle velocity which we explain by an increase in the pressure drop which drags the particles into a denser packing as the flow velocity increases. This counter-intuitive behaviour is the opposite to what is found with Brownian particles, which can reorganize by Brownian motion into denser packing during drying, as long as the flow velocity is not too high. These results show that different kinetic conditions can be used to obtain dense, defect-free regions of particles after drying. In particular, it suggests that rapid, directional drying could be used to control the crystallinity of particle deposits.