Particle Ice Front Interaction - The Brownian Ratchet Model

TL;DR

This paper models particle-ice front interactions as a Brownian ratchet, deriving a relation for particle dragging distance during freezing, which aligns with experimental observations and explains pattern formation in colloidal suspensions.

Contribution

It introduces a stochastic model for particle pushing by ice growth, providing analytical and numerical results for particle engulfment distances and their implications for pattern formation.

Findings

Derived a relation L ~ exp[1/(vr)] for particle dragging distance.

Confirmed the model's predictions with experimental data on ice lenses and lamellae.

Linked particle dynamics to pattern formation in phase transitions.

Abstract

We treat the problem of particle pushing by growing ice as a free diffusion near a wall that moves with discrete steps. When the particle diffuse away from the surface the surface can grow, blocking the particle from going back. Elementary calculations of the model reproduce established results for the critical velocity $v_c$ for particle engulfment: $v_c\sim 1/r$ for large particles and $v_c\sim$ Const for small particles, $r$ being the particle's radius. Using our model we calculate the dragging distance of the particle by treating the pushing as a sequence of growing steps by the surface, each enabled by the particle's diffusion away. Eventually the particle is engulfed by ice growing around it when a rare event of long diffusion time away from the surface occurs. By calculating numerically the statistics of the diffusion times from the surface and therefore the probability for a such a rare event we calculate the total dragging time and distance $L$ of the particle by the ice front to be $L\sim\exp[1/(vr)]$ where $v$ is the freezing velocity. This relation for $L$ is confirmed by ours and others experiments. The distance $L$ provides a length scale for pattern formation during phase transition in colloidal suspensions, such as ice lenses and lamellae structures by freeze casting. Data from the literature for ice lenses thickness and lamellae spacing during freeze casting agree with our prediction for the relation of the distance $L$. These results lead us to conjecture that lamellae formation is dominated by their lateral growth which pushes and concentrates the particles between them.