Rapid shear viscosity calculation by momentum impulse relaxation molecular dynamics

Abstract

Recently, Arya [J. Chem. Phys. 113, 2079 (2000)] introduced a new molecular dynamics method to rapidly compute the viscosity of fluids. The technique, termed momentum impulse relaxation (MIR), involves the imposition of a Gaussian velocity profile on an equilibrated system, after which the decay in the profile is monitored as a function of time. The shear viscosity is computed by matching the rate of decay of the velocity profile to the corresponding solution of the Navier-Stokes equation. The method was originally applied to simple systems (argon and n -butane) and found to give a comparable accuracy to conventional equilibrium and nonequilibrium methods with more than an order of magnitude reduction in computing time. In this work, we extend and generalize the method to examine larger molecules with higher viscosities than have been examined previously. A detailed analysis of the method is given, including the effect the velocity boundary conditions have on the viscosity, the sensitivity of the results to the velocity profile fitting procedure, the effect of preequilibration of the Gaussian profile, and the effect the system size and box shape have on the accuracy and speed of the method. It is shown that the MIR method can be extended to treat multiatom systems without loss of accuracy or computational efficiency. © 2005 American Institute of Physics.