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


A V Lukyanov, A E Likhtman. Relaxation of surface tension in the free-surface boundary layer of simple Lennard-Jones liquids. The Journal of chemical physics. 2013 Jan 21;138(3):034712

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PMID: 23343298

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