Abstract

Molecular simulation is ideally suited to explore and describe the behavior of inhomo-geneous fluid mixtures as it allows a unique perspective into the physics at the scale relevant tointerfacial properties, filling the gaps between experimental determinations and theoretical pre-dictions. Although rather common Molecular Dynamics and Monte Carlo schemes are employed,the technical implementation and the post-processing of the results are more challenging thanfor homogeneous fluids due to the spatial dependence of the interfacial properties. This work isdevoted to describing and recommending methods for molecular-simulation computation of themost important interfacial properties of pure fluids and fluid mixtures,i.e., interfacial concentrationof species, the interfacial thickness, the surface activity or adsorption of species, superficial enthalpyand entropy, wetting between phases and the interfacial or surface tension on planar interfaces.Herein, a detailed description is given of the steps required to perform classical molecular simu-lations including setting up of the initial configuration, choice of cell dimensions, thermodynamicconditions and ensemble, selection of the force field, simulation length, etc. and a discussion ofthe required post-processing steps in order to obtain interfacial properties. Additionally, generalbackground and description of the expected results of interfacial fluid properties are provided,and step-by-step examples are included for the case of interfacial properties of pure fluids (carbondioxide, decane) and mixtures (carbon dioxide + decane).