Dimensional study of the caging order parameter at the glass transition.

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The glass problem is notoriously hard and controversial. Even at the mean-field level, little is agreed upon regarding why a fluid becomes sluggish while exhibiting but unremarkable structural changes. It is clear, however, that the process involves self-caging, which provides an order parameter for the transition. It is also broadly assumed that this cage should have a gaussian shape in the mean-field limit. Here we show that this ansatz does not hold. By performing simulations as a function of spatial dimension d, we find the cage to keep a nontrivial form. Quantitative mean-field descriptions of the glass transition, such as mode-coupling theory, density functional theory, and replica theory, all miss this crucial element. Although the mean-field random first-order transition scenario of the glass transition is qualitatively supported here and non-mean-field corrections are found to remain small on decreasing d, reconsideration of its implementation is needed for it to result in a coherent description of experimental observations.





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Charbonneau, Patrick, Atsushi Ikeda, Giorgio Parisi and Francesco Zamponi (2012). Dimensional study of the caging order parameter at the glass transition. Proc Natl Acad Sci U S A, 109(35). pp. 13939–13943. 10.1073/pnas.1211825109 Retrieved from https://hdl.handle.net/10161/12602.

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Patrick Charbonneau

Professor of Chemistry

Professor Charbonneau studies soft matter. His work combines theory and simulation to understand the glass problem, protein crystallization, microphase formation, and colloidal assembly in external fields.

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