Identifying time scales for violation/preservation of Stokes-Einstein relation in supercooled water

Abstract

The violation of Stokes--Einstein (SE) relation $D\sim (\eta /T{)}^{-1}$ between the shear viscosity $\eta$ and the translational diffusion constant $D$ at temperature $T$ is of great importance for characterizing anomalous dynamics of supercooled water. Determining which time scales play key roles in the SE violation remains elusive without the measurement of $\eta$. Here we provide comprehensive simulation results of the dynamic properties involving $\eta$ and $D$ in TIP4P/2005 supercooled water. This enabled the thorough identification of the appropriate time scales for SE relation $D\eta /T$. In particular, it is demonstrated that the temperature dependence of various time scales associated with structural relaxation, hydrogen bond breakage, stress relaxation, and dynamic heterogeneities can be definitely classified into only two classes. That is, we propose the generalized SE relations that exhibit "violation" or "preservation". The classification depends on the examined time scales that are coupled or decoupled with the diffusion. On the basis of the classification, we explain the physical origins of the violation in terms of the increase in the plateau modulus and the nonexponentiality of stress relaxation. This implies that the mechanism of SE violation is attributed to the attained solidity upon supercooling, which is in accord with the growth of non-Gaussianity and spatially heterogeneous dynamics.

9 pages with 3 figures for main text, 2 pages with 4 figures for supplementary materials, to appear in Science Advances

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