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In this paper we use molecular dynamics (MD) to answer a classical question:how does the surface tension on a liquid/gas interface appear? After definingsurface tension from the first principles and performing several consistencychecks, we perform a dynamic experiment with a single simple liquidnanodroplet. At time zero, we remove all molecules of the interfacial layer,creating a fresh bare interface with the bulk arrangement of molecules. Afterthat the system evolves towards equilibrium, and the expected surface tensionis re-established. We found that the system relaxation consists of threedistinct stages. First, the mechanical balance is quickly re-established.During this process the notion of surface tension is meaningless. In the secondstage, the surface tension equilibrates, and the density profile broadens to avalue which we call "intrinsic" interfacial width. During the third stage, thedensity profile continues to broaden due to capillary wave excitations, whichdoes not however affect the surface tension. We have observed this scenario formonatomic Lennard-Jones (LJ) liquid as well as for binary LJ mixtures atdifferent temperatures, monitoring a wide range of physical observables.

Relaxation of surface tension in the free-surface boundary layer of simple Lennard-Jones liquids