Stochastic Density Functional Theory on Lane Formation in Electric-Field-Driven Ionic Mixtures: Flow-Kernel-Based Formulation

TL;DR

This paper develops a stochastic density functional theory with multiplicative noise to analyze lane formation in electric-field-driven ionic mixtures, linking linear stability analysis with charge correlation functions and domain pattern formation.

Contribution

It extends deterministic dynamical DFT by incorporating stochastic effects, providing a new framework to understand non-equilibrium lane formation in ionic mixtures.

Findings

Derived the stochastic DFT with multiplicative noise for laning phenomena.

Linked linear stability analysis to charge-charge correlation functions.

Demonstrated stripe domain formation through correlation functions and inverse Fourier transforms.

Abstract

Simulation and experimental studies have demonstrated non-equilibrium ordering in driven colloidal suspensions: with increasing driving force, a uniform colloidal mixture transforms into a locally demixed state characterized by the lane formation or the emergence of strongly anisotropic stripe-like domains. Theoretically, we have found that a linear stability analysis of density dynamics can explain the non-equilibrium ordering by adding a non-trivial advection term. This advection arises from fluctuating flows due to non-Coulombic interactions associated with oppositely driven migrations. Recent studies based on the dynamical density functional theory (DFT) without multiplicative noise have introduced the flow kernel for providing a general description of the fluctuating velocity. Here, we assess and extend the above deterministic DFT by treating electric-field-driven binary ionic mixtures as the primitive model. First, we develop the stochastic DFT with multiplicative noise for the laning phenomena. The stochastic DFT considering the fluctuating flows allows us to determine correlation functions in a steady state. In particular, asymptotic analysis on the stationary charge-charge correlation function reveals that the above dispersion relation for linear stability analysis is equivalent to the pole equation for determining the oscillatory wavelength of charge--charge correlations. Next, the appearance of stripe-like domains is demonstrated not only by using the pole equation but also by performing the 2D inverse Fourier transform of the charge--charge correlation function without the premise of anisotropic homogeneity in the electric field direction.