Low Mach Number Fluctuating Hydrodynamics of Multispecies Liquid Mixtures

TL;DR

This paper develops a low Mach number fluctuating hydrodynamics framework for multispecies liquid mixtures, enabling efficient simulation of complex transport phenomena including concentration fluctuations and gravitational instabilities.

Contribution

It generalizes previous models to non-ideal, multi-species mixtures without a solvent, incorporating temperature and pressure gradients, and extends numerical methods for studying nonequilibrium fluctuations.

Findings

Giant nonequilibrium fluctuations can trigger instabilities.

Numerical results agree with experimental measurements.

Fluctuations initially dominate but are overtaken by deterministic growth.

Abstract

We develop a low Mach number formulation of the hydrodynamic equations describing transport of mass and momentum in a multispecies mixture of incompressible miscible liquids at specified temperature and pressure that generalizes our prior work on ideal mixtures of ideal gases and binary liquid mixtures. In this formulation we combine and extend a number of existing descriptions of multispecies transport available in the literature. The formulation applies to non-ideal mixtures of arbitrary number of species, without the need to single out a 'solvent' species, and includes contributions to the diffusive mass flux due to gradients of composition, temperature and pressure. Momentum transport and advective mass transport are handled using a low Mach number approach that eliminates fast sound waves (pressure fluctuations) from the full compressible system of equations and leads to a quasi-incompressible formulation. Thermal fluctuations are included in our fluctuating hydrodynamics description following the principles of nonequilibrium thermodynamics. We extend the semi-implicit staggered-grid finite-volume numerical method developed in our prior work on binary liquid mixtures, and use it to study the development of giant nonequilibrium concentration fluctuations in a ternary mixture subjected to a steady concentration gradient. We also numerically study the development of diffusion-driven gravitational instabilities in a ternary mixture, and compare our numerical results to recent experimental measurements in a Hele-Shaw cell. We find that giant nonequilibrium fluctuations can trigger the instability but are eventually dominated by the deterministic growth of the unstable mode, in both quasi two-dimensional (Hele-Shaw), and fully three-dimensional geometries used in typical shadowgraph experiments.