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Excess wings and asymmetric relaxation spectra in a facilitated trap model. | LitMetric

Excess wings and asymmetric relaxation spectra in a facilitated trap model.

J Chem Phys

Laboratoire Charles Coulomb (L2C), Université de Montpellier, CNRS, 34095 Montpellier, France.

Published: August 2021

In a recent computer study, we have shown that the combination of spatially heterogeneous dynamics and kinetic facilitation provides a microscopic explanation for the emergence of excess wings in deeply supercooled liquids. Motivated by these findings, we construct a minimal empirical model to describe this physics and introduce dynamic facilitation in the trap model, which was initially developed to capture the thermally activated dynamics of glassy systems. We fully characterize the relaxation dynamics of this facilitated trap model varying the functional form of energy distributions and the strength of dynamic facilitation, combining numerical results and analytic arguments. Dynamic facilitation generically accelerates the relaxation of the deepest traps, thus making relaxation spectra strongly asymmetric, with an apparent "excess" signal at high frequencies. For well-chosen values of the parameters, the obtained spectra mimic experimental results for organic liquids displaying an excess wing. Overall, our results identify the minimal physical ingredients needed to describe excess processes in the relaxation spectra of supercooled liquids.

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Source
http://dx.doi.org/10.1063/5.0060408DOI Listing

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