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.
Molecular Dynamics Simulation
Published Version (Please cite this version)10.1073/pnas.1211825109
Publication InfoCharbonneau, Patrick; Ikeda, A; Parisi, G; & Zamponi, Francesco (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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Associate 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.