However, they might break down at low temperature. These relations are indeed obeyed by many liquids at sufficiently high temperature. If objects as small as molecules were to follow macroscopic hydrodynamics, one would expect that the preceding quantities would be related through the Stokes–Einstein (SE), D t ∝ T / η, and Stokes–Einstein–Debye (SED), D r ∝ T / η, relations, where T is the temperature. In usual glassformers, many studies have focused on the coupling or decoupling between the following dynamic quantities: viscosity ( η) and self or tracer diffusion coefficients for translation ( D t) and rotation ( D r). This idea has motivated experimental efforts to measure dynamic properties of supercooled water and has received some indirect support from experiments on nanoconfined water ( 18– 20) and from simulations ( 21, 22). Based on these and other observations, it has been hypothesized that supercooled water experiences a fragile-to-strong transition ( 17). The temperature dependence of the relaxation time is well described by a power law ( 8, 9), as expected from mode-coupling theory ( 15, 16), which usually applies well to liquids with a small change of sound velocity upon vitrification. However, pioneering measurements on bulk supercooled water by NMR ( 11) and quasi-elastic neutron scattering ( 12), as well as recent ones by optical Kerr effect ( 8, 9), reveal a large super-Arrhenius behavior between 340 and 240 K, similar to what is observed in fragile glassformers ( 13, 14). Such a large jump is usually the signature of a strong glass, i.e., one in which relaxation times or viscosity follow an Arrhenius law upon cooling. Indeed, whereas the sound velocity is around 1,400 m ⋅ s − 1 in liquid water at 273 K, it reaches around 3,300 m ⋅ s − 1 in ice at 273 K and a similar value in the known amorphous phases of ice at 80 K ( 10). Although the viscosity of water strongly decouples from translational motion, a scaling with rotational motion remains, similar to canonical glassformers.Īs an example, crystallization of water is accompanied by one of the largest known relative changes in sound velocity, which has been attributed to the relaxation effects of the hydrogen bond network ( 8, 9). In molecular glassformers or liquid metals, the violation of the Stokes–Einstein relation signals the onset of spatially heterogeneous dynamics and collective motions. Our results allow us to test the Stokes–Einstein and Stokes–Einstein–Debye relations that link viscosity, a macroscopic property, to the molecular translational and rotational diffusion, respectively. A single power law reproduces the 50-fold variation of viscosity up to the boiling point. Here we report viscosity of water supercooled close to the limit of homogeneous crystallization. Water is a notoriously poor glassformer, and the supercooled liquid crystallizes easily, making the measurement of its viscosity a challenging task. Viscosity increases dramatically upon cooling, until dynamical arrest when a glassy state is reached. The viscosity of a liquid measures its resistance to flow, with consequences for hydraulic machinery, locomotion of microorganisms, and flow of blood in vessels and sap in trees.
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