arXiv subjects

Peter J. Daivis

Publications and source records attributed to Peter J. Daivis.

5 recordsLinked to original sources

arXiv2025

The influence of boundary conditions and interfacial slip on the time taken to achieve a nonequilibrium steady-state for highly confined flows

We investigate the equilibration time to attain steady-state for a system of liquid molecules under boundary-driven planar Couette flow via nonequilibrium molecular dynamics (NEMD) simulation. In particular, we examine the equilibration time for the two common types of boundary driven flow: one in which both walls slide with equal and opposite velocity, and the other in which one wall is fixed and the other moves with twice the velocity. Both flows give identical steady-state strain rates, and hence flow properties, but the transient behaviour is completely different. We find that in the case of no-slip boundary conditions, the equilibration times for the counter-sliding walls flow are exactly 4 times faster than those of the single sliding wall system, and this is independent of the atomistic nature of the fluid, i.e., it is an entirely hydrodynamic feature. We also find that systems that exhibit slip have longer equilibration times in general and the ratio of equilibration times for the two types of boundary-driven flow is even more pronounced. We analyse the problem by decomposing a generic planar Couette flow into a linear sum of purely symmetric and antisymmetric flows. We find that the no-slip equilibration time is dominated by the slowest decaying eigenvalue of the solution to the Navier-Stokes equation. In the case of slip, the longest relaxation time is now dominated by the transient slip velocity response, which is longer than the no-slip response time. In the case of a high-slip system of water confined to graphene channels, the enhancement is over two orders of magnitude.

physics.flu-dyn↗

arXiv2023

TTCF4LAMMPS: A toolkit for simulation of the non-equilibrium behaviour of molecular fluids at experimentally accessible shear rates

We present TTCF4LAMMPS, a toolkit for performing non-equilibrium molecular dynamics (NEMD) simulations to study fluid behaviour at low shear rates using the LAMMPS software. By combining direct NEMD simulations and the transient-time correlation function (TTCF) technique, we study the behaviour of fluids over shear rates spanning $15$ orders of magnitude. We present two example systems consisting of simple monatomic systems: one containing a bulk liquid and another with a liquid layer confined between two solid walls. The small bulk system is suitable for testing on personal computers, while the larger confined system requires high-performance computing (HPC) resources. We demonstrate that the TTCF formalism can successfully detect the system response for arbitrarily weak external fields. We provide a brief mathematical explanation for this feature. Although we showcase the method for simple monatomic systems, TTCF can be readily extended to study more complex molecular fluids. Moreover, in addition to shear flows, the method can be extended to investigate elongational or mixed flows as well as thermal or electric fields. The reasonably high computational cost needed for the method is offset by the two following benefits: i) the cost is independent of the magnitude of the external field, and ii) the simulations can be made highly efficient on HPC architectures by exploiting the parallel design of LAMMPS. We expect the toolkit to be useful for computational researchers striving to study the nonequilibrium behaviour of fluids under experimentally-accessible conditions.

cond-mat.soft↗

arXiv2022

Slip and Stress From Low Strain-Rate Nonequilibrium Molecular Dynamics: The Transient-Time Correlation Function Technique

We derive the transient-time correlation function (TTCF) expression for the computation of phase variables of inhomogenous confined atomistic fluids undergoing boundary-driven planar shear (Couette) flow at constant pressure. Using nonequilibrium molecular dynamics simulations, we then apply the TTCF formalism to the computation of the shear stress and the slip velocity for atomistic fluids at realistic low shear rates, in systems under constant pressure and constant volume. We show that, compared to direct averaging of multiple trajectories, the TTCF method dramatically improves the accuracy of the results at low shear rates, and that it is suitable to investigate the tribology and rheology of atomistically detailed confined fluids at realistic flow rates.

cond-mat.soft↗

arXiv2015

Continuum Nanofluidics

This paper introduces the fundamental continuum theory governing momentum transport in isotropic nanofluidic flows. The theory is an extension to the classical Navier-Stokes equation, which includes coupling between translational and rotational degrees of freedom, as well as non-local response functions that incorporates spatial correlations. The continuum theory is compared with molecular dynamics simulation data for both relaxation processes and fluid flows showing excellent agreement on the nanometer length scale. We also present practical tools to estimate when the extended theory should be used.

cond-mat.soft↗

arXiv2015

Non-Newtonian behavior and molecular structure of Cooee bitumen under shear flow: a non-equilibrium molecular dynamics study

The rheology and molecular structure of a model bitumen (Cooee bitumen) under shear are investigated in the non-Newtonian regime using non-equilibrium molecular dynamics simulations. The shear viscosity, normal stress differences and pressure of the bitumen mixture are computed at different shear rates and different temperatures. The model bitumen is shown to be a shear-thinning fluid at all temperatures. In addition, the Cooee model is able to reproduce experimental results showing the formation of nanoaggregates composed of stacks of flat aromatic molecules in bitumen. These nanoaggregates are immersed in a solvent of saturated hydrocarbon molecules. At a fixed temperature, the shear-shinning behavior is related to the inter- and intramolecular alignment of the solvent molecules, but also to the decrease of the average size of the nanoaggregates at high shear rates. The variation of the viscosity with temperature at different shear rates is also related to the size and relative composition of the nanoaggregates. The slight anisotropy of the whole sample due to the nanoaggregates is considered and quantified. Finally, the position of bitumen mixtures in the broad literature of complex systems such as colloidal suspensions, polymer solutions and associating polymer networks is discussed.

physics.chem-ph↗