Document Type

Article

Publication Date

August 2018

Publication Title

The Journal of Chemical Physics

Volume

149

Issue Number

8

DOI

10.1063/1.5043428

Disciplines

Other Astrophysics and Astronomy | Other Physics | Physical Sciences and Mathematics

Abstract

Fluctuating hydrodynamics (FHD) provides a framework for modeling microscopic fluctuations in a manner consistent with statistical mechanics and nonequilibrium thermodynamics. This paper presents an FHD formulation for isothermal reactive incompressible liquid mixtures with stochastic chemistry. Fluctuating multispecies mass diffusion is formulated using a Maxwell–Stefan description without assuming a dilute solution, and momentum dynamics is described by a stochastic Navier–Stokes equation for the fluid velocity. We consider a thermodynamically consistent generalization for the law of mass action for non-dilute mixtures and use it in the chemical master equation (CME) to model reactions as a Poisson process. The FHD approach provides remarkable computational efficiency over traditional reaction-diffusion master equation methods when the number of reactive molecules is large, while also retaining accuracy even when there are as few as ten reactive molecules per hydrodynamic cell. We present a numerical algorithm to solve the coupled FHD and CME equations and validate it on both equilibrium and nonequilibrium problems. We simulate a diffusively driven gravitational instability in the presence of an acid-base neutralization reaction, starting from a perfectly flat interface. We demonstrate that the coupling between velocity and concentration fluctuations dominates the initial growth of the instability.

Comments

This is the Version of Record of an article that appeared in The Journal of Chemical Physics, volume 149, issue 8, 2018. The Version of Record (VOR) can also be found at https://doi.org/10.1063/1.5043428
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