Assessment of elastic models in supercooled water: A molecular dynamics study with the TIP4P/2005f force field

Abstract

Glass formers exhibit a viscoelastic behavior: at the laboratory timescale, they behave like (glassy) solids at low temperatures, and like liquids at high temperatures. Based on this observation, elastic models relate the long time supercooled dynamics to short time elastic properties of the supercooled liquid. In the present work, we assess the validity of elastic models for the shear viscosity and the $\alpha$-relaxation time of supercooled water, using molecular dynamics simulations with the TIP4P/2005f force field over a wide range of temperatures. We show that elastic models provide a good description of supercooled water dynamics. For the viscosity, two different regimes are observed and the crossover temperature is found to be close to the one where the Stokes-Einstein relation starts to be violated. Our simulations show that only shear properties are important to characterize the effective flow activation energy. This study calls for experimental determination of the high frequency elastic properties of water at low temperatures.

References in corpus (7)

• Perspective: How good is DFT for water?
• The Individual and Collective Effects of Exact Exchange and Dispersion Interactions on the Ab Initio Structure of Liquid Water
• The first principles calculation of transport coefficients
• Landscape equivalent of the shoving model
• The instantaneous shear modulus in the shoving model
• Universal divergenceless scaling between structural relaxation and caged dynamics in glass-forming systems
• Elastic models of the glass transition applied to a liquid with density anomalies

Cited by in corpus (8)

• Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulations
• Spurious violation of the Stokes-Einstein-Debye relation in supercooled water
• Molecular layers in thin supported films exhibit the same scaling as the bulk between slow relaxation and vibrational dynamics
• Fast dynamics perspective on the breakdown of the Stokes-Einstein law in fragile glassformers
• Classification of mobile- and immobile-molecule timescales for the Stokes-Einstein and Stokes-Einstein-Debye relations in supercooled water
• Fast Vibrational Modes and Slow Heterogeneous Dynamics in Polymers and Viscous Liquids
• Understanding Dynamics in Coarse-Grained Models: IV. Connection of Fine-Grained and Coarse-Grained Dynamics with the Stokes-Einstein and Stokes-Einstein-Debye Relations
• Reliable Viscosity Calculation from High-Pressure Equilibrium Molecular Dynamics: Case Study of 2,2,4-Trimethylhexane