Bottom-up construction of dynamic density functional theories for inhomogeneous polymer systems from microscopic simulations

Abstract

We propose and compare different strategies to construct dynamic density functional theories (DDFTs) for inhomogeneous polymer systems close to equilibrium from microscopic simulation trajectories. We focus on the systematic construction of the mobility coefficient, $\Lambda (r,r^{\prime })$, which relates the thermodynamic driving force on monomers at position $r^{\prime }$ to the motion of monomers at position $r$. A first approach based on the Green-Kubo formalism turns out to be impractical because of a severe plateau problem. Instead, we propose to extract the mobility coefficient from an effective characteristic relaxation time of the single chain dynamic structure factor. To test our approach, we study the kinetics of ordering and disordering in diblock copolymer melts. The DDFT results are in very good agreement with the data from corresponding fine-grained simulations.

Some typos corrected compared to published version (Eqs. (32) and (38))

References in corpus (2)

• Spontaneous formation of complex micelles from homogeneous solution
• Iterative Reconstruction of Memory Kernels

Cited by in corpus (6)

• Classical dynamical density functional theory: from fundamentals to applications
• Perspective: New directions in dynamical density functional theory
• Dynamic self-consistent field approach for studying kinetic processes in multiblock copolymer melts
• Relaxation Dynamics of Entangled Linear Polymer Melts via Molecular Dynamics Simulations
• Dynamic coarse-graining of polymer systems using mobility functions
• The Process-Directed Self-Assembly of Block Copolymer Particles