Can we approach the gas-liquid critical point using slab simulations of two coexisting phases?

Abstract

In this paper, we demonstrate that it is possible to approach the gas-liquid critical point of the Lennard-Jones fluid by performing simulations in a slab geometry using a cut-off potential. In the slab simulation geometry, it is essential to apply an accurate tail correction to the potential energy, applied during the course of the simulation, to study the properties of states close to the critical point. Using the Janeček slab-based method developed for two-phase Monte Carlo simulations [J. Janec̆ek, J. Chem. Phys. 131, 6264 (2006)], the coexisting densities and surface tension in the critical region are reported as a function of the cutoff distance in the intermolecular potential. The results obtained using slab simulations are compared with those obtained using grand canonical Monte Carlo simulations of isotropic systems and the finite-size scaling techniques. There is a good agreement between these two approaches. The two-phase simulations can be used in approaching the critical point for temperatures up to 0.97 TC∗ (T∗ = 1.26). The critical-point exponents describing the dependence of the density, surface tension, and interfacial thickness on the temperature are calculated near the critical point.