Effect of total and pair configurational entropy in determining dynamics of supercooled liquids over a range of densities

A Banerjee and MK Nandi and S Sastry and SM Bhattacharyya, JOURNAL OF CHEMICAL PHYSICS, 145, 034502 (2016).

DOI: 10.1063/1.4958627

In this paper, we present a study of supercooled liquids interacting with the Lennard Jones potential and the corresponding purely repulsive (Weeks-Chandler-Andersen) potential, over a range of densities and temperatures, in order to understand the origin of their different dynamics in spite of their structures being similar. Using the configurational entropy as the thermodynamic marker via the Adam Gibbs relation, we show that the difference in the dynamics of these two systems at low temperatures can be explained from thermodynamics. At higher densities both the thermodynamical and dynamical difference between these model systems decrease, which is quantitatively demonstrated in this paper by calculating different parameters. The study also reveals the origin of the difference in pair entropy despite the similarity in the structure. Although the maximum difference in structure is obtained in the partial radial distribution function of the B type of particles, the rdf of AA pairs and AB pairs gives rise to the differences in the entropy and dynamics. This work supports the observation made in an earlier study A. Banerjee et al., Phys. Rev. Lett. 113, 225701 (2014) and shows that they are generic in nature, independent of density. Published by AIP Publishing.

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