Topological Characterization of Rigid-Nonrigid Transition across the Frenkel Line

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Abstract

The dynamics of supercritical fluids, a state of matter beyond the gas-liquid critical point, changes from diffusive to oscillatory motions at high pressure. This transition is believed to occur across a locus of thermodynamic states called the Frenkel line. The Frenkel line has been extensively investigated from the viewpoint of the dynamics, but its structural meaning is still not well-understood. This Letter interprets the mesoscopic picture of the Frenkel line entirely based on a topological and geometrical framework. This discovery makes it possible to understand the mechanism of rigid-nonrigid transition based not on the dynamics of individual atoms but on their instantaneous configurations. The topological classification method reveals that the percolation of solid-like structures occurs above the rigid-nonrigid crossover densities.

Original languageEnglish
Pages (from-to)6524-6528
Number of pages5
JournalJournal of Physical Chemistry Letters
Volume9
Issue number22
DOIs
StatePublished - 15 Nov 2018
Externally publishedYes

Bibliographical note

Publisher Copyright:
Copyright © 2018 American Chemical Society.

Funding

E.A.L. gratefully acknowledges the generous support of the U.S. National Science Foundation through Award DMR-1507013. W.B.L. and M.Y.H. acknowledge the support of the National Research Foundation of Korea Grants funded by the Korean Government (NRF-2015R1A5A1036133, NRF-2017H1A2A1044355).

FundersFunder number
National Science FoundationDMR-1507013, 1507013
National Research Foundation of KoreaNRF-2017H1A2A1044355, NRF-2015R1A5A1036133

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