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Dynamical Behavior Near a Liquid–Liquid Phase Transition in Simulations of Supercooled Water

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Peter H. Poole*†, Stephen R. Becker‡, Francesco Sciortino*¶, and Francis W. Starr*‡

Department of Physics, St. Francis Xavier University, Antigonish, Nova Scotia B2G 2W5, Canada,

Department of Physics, Wesleyan University, Middletown, Connecticut 06459, United States

Dipartimento di Fisica and CNR-ISC, Università di Roma La Sapienza, Piazzale Aldo Moro 2, I-00185 Rome, Italy

J. Phys. Chem. B, 2011, 115 (48), pp 14176–14183

DOI: 10.1021/jp204889m

Publication Date (Web): August 26, 2011

E-mail: P.H.P., ppoole@stfx.ca; F.S., francesco.sciortino@uniroma1.it; F.W.S., fstarr@wesleyan.edu.

This article is part of the

H. Eugene Stanley Festschrift

special issue.

Section:

General Physical Chemistry

Abstract

We examine the behavior of the diffusion coefficient of the ST2 model of water over a broad region of the phase diagram via molecular dynamics simulations. The ST2 model has an accessible liquid–liquid transition between low-density and high-density phases, making the model an ideal candidate to explore the impacts of the liquid–liquid transition on dynamics. We locate characteristic dynamical loci in the phase diagram and compare them with the previously investigated thermodynamic loci. The low-density liquid phase shows a crossover from non-Arrhenius to Arrhenius behavior, signaling the onset of a crossover from fragile-to-strong behavior. We explain this crossover in terms of the asymptotic approach of the low-density liquid to a random tetrahedral network and show that the temperature dependence of the diffusion coefficient over a wide temperature range can be simply related to the concentration of defects in the network. Our findings thus confirm that the low-density phase of ST2 water is a well-defined metastable liquid.

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