The frequency dependent shear viscosity of methane

Accurate computer simulation calculations of hydrodynamic transport coefficients are notoriously expensive. In this paper we develop a method based on the non-equilibrium molecular dynamics of Ashurst and Hoover [1] which calculates the spectrum of stress-stress correlation with greater efficiency than has hitherto been possible. The calculation shows that a potential function for methane, due to Williams [2], predicts a zero frequency shear viscosity within 10 per cent of the experimental value. The spectrum of stress-stress correlation gives clear evidence of a t -3/2 long-time tail. It is shown that the spectrum is not a monotonic decreasing function of frequency. This has not been seen in computer simulation before but is in agreement with the mode-coupling prediction of Bosse et al. [3].

[1]  Donald E. Williams.  Nonbonded Potential Parameters Derived from Crystalline Hydrocarbons , 1967 .

[2]  W. Hoover,et al.  Argon Shear Viscosity via a Lennard-Jones Potential with Equilibrium and Nonequilibrium Molecular Dynamics , 1973 .

[3]  Denis J. Evans,et al.  On the representatation of orientation space , 1977 .

[4]  William B. Streett,et al.  Transport properties of homonuclear diatomics , 1978 .

[5]  L. Verlet,et al.  Computer "Experiments" on Classical Fluids. IV. Transport Properties and Time-Correlation Functions of the Lennard-Jones Liquid near Its Triple Point , 1973 .

[6]  Gustav Doetsch,et al.  Guide to the applications of Laplace transforms , 1961 .

[7]  W. M. Haynes,et al.  Equations for the viscosity and thermal conductivity coefficients of methane , 1975 .

[8]  I. R. Mcdonald,et al.  Theory of simple liquids , 1998 .

[9]  D. Evans.  The nonsymmetric pressure tensor in polyatomic fluids , 1979 .

[10]  I. R. Mcdonald,et al.  On the calculation by molecular dynamics of the shear viscosity of a simple fluid , 1973 .

[11]  L. Verlet.  Computer "Experiments" on Classical Fluids. I. Thermodynamical Properties of Lennard-Jones Molecules , 1967 .

[12]  N. H. March,et al.  Non-analyticity of frequency spectra in classical liquids , 1970 .

[13]  G. Ciccotti,et al.  Direct Computation of Dynamical Response by Molecular Dynamics: The Mobility of a Charged Lennard-Jones Particle , 1975 .

[14]  R. H. Silsbee,et al.  The Physics of Solids , 1964 .

[15]  G. Ciccotti,et al.  Transport properties of molten alkali halides , 1976 .

[16]  D. Evans.  On the generalized hydrodynamics of polyatomic fluids , 1976 .

[17]  B. Alder,et al.  Decay of Time Correlations in Two Dimensions , 1971 .

[18]  R. Kiehn,et al.  Neutron Inelastic Scattering , 1954 .

[19]  W. Götze,et al.  Mode-coupling theory of simple classical liquids , 1978 .

[20]  F. Stillinger,et al.  Improved simulation of liquid water by molecular dynamics , 1974 .

[21]  Sohail Murad,et al.  Singularity free algorithm for molecular dynamics simulation of rigid polyatomics , 1977 .

[22]  R. Haymaker.  PHASE SHIFTS FROM THE BETHE--SALPETER DIFFERENTIAL EQUATION. , 1967 .

[23]  Pierre Resibois,et al.  Time dependent correlation functions and mode-mode coupling theories , 1975 .

[24]  T. Naitoh,et al.  The shear viscosity of hard-sphere fluid via non-equilibrium molecular dynamics , 1976 .