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      Perspective: Configurational entropy of glass-forming liquids

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          Abstract

          The configurational entropy is one of the most important thermodynamic quantities characterizing supercooled liquids approaching the glass transition. Despite decades of experimental, theoretical, and computational investigation, a widely accepted definition of the configurational entropy is missing, its quantitative characterization remains fraud with difficulties, misconceptions and paradoxes, and its physical relevance is vividly debated. Motivated by recent computational progress, we offer a pedagogical perspective on the configurational entropy in glass-forming liquids. We first explain why the configurational entropy has become a key quantity to describe glassy materials, from early empirical observations to modern theoretical treatments. We explain why practical measurements necessarily require approximations that make its physical interpretation delicate. We then demonstrate that computer simulations have become an invaluable tool to obtain precise, non-ambiguous, and experimentally-relevant measurements of the configurational entropy. We describe a panel of available computational tools, offering for each method a critical discussion. This perspective should be useful to both experimentalists and theoreticians interested in glassy materials and complex systems.

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          Most cited references 109

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          On the Temperature Dependence of Cooperative Relaxation Properties in Glass‐Forming Liquids

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            Scaling concepts for the dynamics of viscous liquids near an ideal glassy state

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                Author and article information

                Journal
                20 February 2019
                Article
                1902.07679

                http://arxiv.org/licenses/nonexclusive-distrib/1.0/

                Custom metadata
                20 pages, 11 figures, submitted to the Journal of Chemical Physics
                cond-mat.stat-mech cond-mat.dis-nn cond-mat.soft

                Condensed matter, Theoretical physics

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