Unraveling the success and failure of mode coupling theory from consideration of entropy

Abstract

We analyze the dynamics of model supercooled liquids in a temperature regime where predictions of mode coupling theory (MCT) are known to be valid qualitatively. In this regime, the Adam-Gibbs (AG) relation, based on an activation picture of dynamics also describes the dynamics satisfactorily, and we explore the mutual consistency and interrelation of these descriptions. Although entropy and dynamics are related via phenomenological theories, the connection between MCT and entropy has not been argued for. In this work we explore this connection and provide a microscopic derivation of the phenomenological Rosenfeld theory. At low temperatures the overlap between MCT power law regime and AG relation implies that the AG relation predicts an avoided divergence at $T_c$, the origin of which is traced back to the vanishing of pair configurational entropy, which we find occurs at the same temperature. We also show that the residual multiparticle entropy plays an important role in describing the relaxation time

25 pages ,8 figures

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• Effect of total and pair configurational entropy in determining dynamics of supercooled liquids over a range of densities
• Understanding Dynamics in Coarse-Grained Models: II. Coarse-Grained Diffusion Modeled Using Hard Sphere Theory
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• Understanding Dynamics in Coarse-Grained Models: V. Extension of Coarse-Grained Dynamics Theory to Non-Hard Sphere Systems
• Finite-size excess-entropy scaling for simple liquids
• Structure-Dynamics Correlation and Its Link to Fragility and Dynamic Heterogeneity
• Connection between water's dynamical and structural properties: insights from ab initio simulations