Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 115, Issue 38, Pages 9444-9449Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1807821115
Keywords
water's anomalies; structural origin; two-state model; fragile-to-strong transition; dynamic heterogeneity
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Funding
- Japan Society for the Promotion of Science [21224011, 25000002, 18H03675]
- European Research Council [DLV-759187]
- Royal Society University Research Fellowship
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Liquids can be broadly classified into two categories, fragile and strong ones, depending on how their dynamical properties change with temperature. The dynamics of a strong liquid obey the Arrhenius law, whereas the fragile one displays a super-Arrhenius law, with a much steeper slowing down upon cooling. Recently, however, it was discovered that many materials such as water, oxides, and metals do not obey this simple classification, apparently exhibiting a fragile-to-strong transition far above T-g. Such a transition is particularly well known for water, and it is now regarded as one of water's most important anomalies. This phenomenon has been attributed to either an unusual glass transition behavior or the crossing of a Widom line emanating from a liquid-liquid critical point. Here by computer simulations of two popular water models and through analyses of experimental data, we show that the emergent fragile-to-strong transition is actually a crossover between two Arrhenius regimes with different activation energies, which can be naturally explained by a two-state description of the dynamics. Our finding provides insight into the fragile-to-strong transition observed in a wide class of materials.
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