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arXiv · 1206.3915

Dependence of the fragility of a glass former on the softness of interparticle interactions

Shiladitya Sengupta·Filipe Vasconcelos·Frédéric Affouard·Srikanth Sastry
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Abstract

We study the influence of the softness of the interparticle interactions on the fragility of a glass former, by considering three model binary mixture glass formers. The interaction potential between particles is a modified Lennard-Jones type potential, with the repulsive part of the potential varying with an inverse power $q$ of the interparticle distance, and the attractive part varying with an inverse power $p$. We consider the combinations (12,11) (model I), (12,6) (model II) and (8,5) (model III) for (q,p) such that the interaction potential becomes softer from model I to III. We evaluate the kinetic fragilities from the temperature variation of diffusion coefficients and relaxation times, and a thermodynamic fragility from the temperature variation of the configuration entropy. We find that the kinetic fragility increases with increasing softness of the potential, consistent with previous results for these model systems, but at variance with the thermodynamic fragility, which decreases with increasing softness of the interactions, as well as expectations from earlier results. We rationalize our results by considering the full form of the Adam-Gibbs relation, which requires, in addition to the temperature dependence of the configuration entropy, knowledge of the high temperature activation energies ino rder to determine fragility. We show that consideration of the scaling of the high temperature activation energy with the liquid density, analyzed in recent studies, provides a partial rationalization of the observed behavior.

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Shiladitya Sengupta, Filipe Vasconcelos, Frédéric Affouard, Srikanth Sastry. 2012-06-18. Dependence of the fragility of a glass former on the softness of interparticle interactions. https://doi.org/10.1063/1.3660201

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