Equilibrium and Non-equilibrium Molecular Dynamics Simulations of Thermal Transport Coefficients of Liquid Argon

摘要

The thermal transport coefficients-the self-diffusion coefficient, shear viscosity, and thermal conductivity-of liquid argon at 94.4 K and 1 atm are calculated by non-equilibrium molecular dynamics (NEMD) simulations of a Lennard-Jones potential and compared with those obtained from Green-Kubo relations using equilibrium molecular dynamics (EMD) simulations and with experimental data. The time-correlation functions-the velocity, pressure, and heat flux auto-correlation functions-of liquid argon obtained from the EMD simulations show well-behaved smooth curves which are not oscillating and decaying fast around 1.5 ps. The calculated self-diffusion coefficient from our NEMD simulation is found to be approximately 40% higher than the experimental result. The Lagrange extrapolated shear viscosity is in good agreement with the experimental result and the asymptotic formula of the calculated shear viscosities seems to be an exponential form rather than the square-root form predicted by other NEMD studies of shear viscosity. The agreement for thermal conductivity between the simulation results (NEMD and EMD) and the experimental result is within statistical error. In conclusion, through our NEMD and EMD simulations, the overall agreement is quite good, which means that the Green-Kubo relations and the NEMD algorithms of thermal transport coefficients for simple liquids are valid.