A hybrid method coupling fluctuating hydrodynamics and molecular dynamics for the simulation of macromolecules

TL;DR

This paper introduces a hybrid simulation method combining fluctuating hydrodynamics and molecular dynamics to accurately model macromolecular behavior in solution, capturing static and dynamic properties consistent with established models.

Contribution

The authors develop a novel hybrid computational approach coupling fluctuating hydrodynamics with molecular dynamics, improving the simulation of polymer dynamics and fluid interactions.

Findings

Accurately reproduces static conformations of polymers.

Matches the Zimm model's predictions for diffusion and viscosity.

Identifies the limitations of Zimm model at low Schmidt numbers.

Abstract

We present a hybrid computational method for simulating the dynamics of macromolecules in solution which couples a mesoscale solver for the fluctuating hydrodynamics (FH) equations with molecular dynamics to describe the macromolecule. The two models interact through a dissipative Stokesian term first introduced by Ahlrichs and D\"unweg [J. Chem. Phys. {\bf 111}, 8225 (1999)]. We show that our method correctly captures the static and dynamical properties of polymer chains as predicted by the Zimm model. In particular, we show that the static conformations are best described when the ratio $\frac{\sigma}{b}=0.6$, where $\sigma$ is the Lennard-Jones length parameter and $b$ is the monomer bond length. We also find that the decay of the Rouse modes' autocorrelation function is better described with an analytical correction suggested by Ahlrichs and D\"unweg. Our FH solver permits us to treat the fluid equation of state and transport parameters as direct simulation parameters. The expected independence of the chain dynamics on various choices of fluid equation of state and bulk viscosity is recovered, while excellent agreement is found for the temperature and shear viscosity dependence of centre of mass diffusion between simulation results and predictions of the Zimm model. We find that Zimm model approximations start to fail when the Schmidt number $Sc \lessapprox 30$. Finally, we investigate the importance of fluid fluctuations and show that using the preaveraged approximation for the hydrodynamic tensor leads to around 3% error in the diffusion coefficient for a polymer chain when the fluid discretization size is greater than $50\AA$.