Relative entropy indicates an ideal concentration for structure-based coarse graining of binary mixtures

D Rosenberger and NFA van der Vegt, PHYSICAL REVIEW E, 99, 053308 (2019).

DOI: 10.1103/PhysRevE.99.053308

Many methodological approaches have been proposed to improve systematic or bottom-up coarse-graining techniques to enhance the representability and transferability of the derived interaction potentials. Transferability describes the ability of a coarse-grained (CG) model to be predictive, i.e., to describe a system at state points different from those chosen for parametrization. Whereas the representability characterizes the accuracy of a CG model to reproduce target properties of the underlying reference or fine-grained model at a given state point. In this article, we shift the focus away from methodological aspects and rather raise the question whether we can overcome the disadvantages of a given method in terms of representability and transferability by systematically selecting the state point at which the CG model gets parametrized. We answer this question by applying the inverse Monte Carlo (IMC) approach-a structure-based coarse-graining method-to derive effective interactions for binary mixtures of simple Lennard-Jones (LJ) particles, which are different in size. For such simple systems we indeed can identify a concentration where the derived potentials show the best performance in terms of structural representability and transferability. This specific concentration is identified by computing the relative entropy which quantifies the information loss between different IMC models and the reference LJ model at varying mixture compositions. Further, we show that an IMC model for mixtures of n-hexane and n-perfluorohexane shows the same trend in transferability as the IMC models for the LJ system. All derived models are more transferable in the direction of increasing concentration of the larger-sized compound.

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