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An Analog Macroscopic Technique for Studying Molecular Hydrodynamic Processes in Dense Gases and Liquids

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Dynamical density functional theory and its application to spinodal decomposition.

A J Archer¹, R Evans

¹H.H. Wills Physics Laboratory, University of Bristol, Bristol BS8 1TL, United Kingdom. andrew.archer@bristol.ac.uk

The Journal of Chemical Physics

|August 31, 2004

Summary

We present a new derivation of dynamical density functional theory (DDFT) applicable to complex fluids with multibody interactions. This DDFT approach extends to model spinodal decomposition beyond current theories.

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Area of Science:

Statistical Mechanics
Soft Matter Physics
Physical Chemistry

Background:

Dynamical density functional theory (DDFT) is crucial for understanding classical fluids.
Existing DDFT models often assume pair potentials, limiting their applicability.
Spinodal decomposition is a key process in phase transitions of fluids.

Purpose of the Study:

To provide an alternative derivation of DDFT for classical fluids.
To extend DDFT to systems with multibody interactions.
To develop a DDFT-based theory for spinodal decomposition applicable at early and intermediate times.

Main Methods:

Derivation of DDFT starting from the Smoluchowski equation.
Application of the derived DDFT to model spinodal decomposition.
Analysis of density fluctuations and mode coupling in fluids.

Main Results:

The derived DDFT is valid for general multibody interactions, not just pair potentials.
The theory successfully describes spinodal decomposition beyond the Cahn-Hilliard theory.
Calculations reveal coupling of density fluctuation modes, leading to a secondary peak in fluctuations.

Conclusions:

The generalized DDFT offers a more comprehensive framework for classical fluids.
The new spinodal decomposition theory captures complex dynamics beyond linear approximations.
This work provides new insights into phase separation mechanisms in colloidal and complex fluids.