Thermal Offset Viscosities of Liquid H2O, D2O, and T2O

Cho, C. H.; Urquidi, Jacob; Singh, and S.; Robinson, G. W.

doi:10.1021/jp9842953

Cited by 256 publications

(254 citation statements)

References 25 publications

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“…These extend to 238 K for co-workers, 13 who used 1 m capillaries. However consistent t values are obtained for the two isotopomers, 0.668, and, as noted in our original paper, the transition temperature difference is consistent with the thermal offset noted by Robinson and co-workers 14 for the two transport properties. 15 The transition temperatures are rather higher than other estimates that have been used to support arguments for dynamic heterogeneities in supercooled water.…”

supporting

confidence: 91%

Communications: The fractional Stokes–Einstein equation: Application to water

Harris

2010

The Journal of Chemical Physics

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supporting

confidence: 91%

Communications: The fractional Stokes–Einstein equation: Application to water

Harris

2010

The Journal of Chemical Physics

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“…Good agreement is found for the stable liquid above 273 K. We confirm Hallett's measurements on supercooled water (43) and extend them by 10 K. We find however systematically lower values than Osipov et al (44) at low temperature. Referring to previous work (47) showing an increase of the density of water inside small μm-sized capillaries, Cho et al (45) argued that this effect might have changed the viscosity of water in the experiment of Osipov et al, who used quartz capillaries with radius R = 1 μm. We propose another possible bias: electroosmosis.…”

Section: Resultsmentioning

confidence: 91%

Viscosity of deeply supercooled water and its coupling to molecular diffusion

Dehaoui

Issenmann

Caupin

2015

Proc. Natl. Acad. Sci. U.S.A.

204

213

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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. Viscosity increases dramatically upon cooling, until dynamical arrest when a glassy state is reached. Water is a notoriously poor glassformer, and the supercooled liquid crystallizes easily, making the measurement of its viscosity a challenging task. Here we report viscosity of water supercooled close to the limit of homogeneous crystallization. Our values contradict earlier data. A single power law reproduces the 50-fold variation of viscosity up to the boiling point. 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. In molecular glassformers or liquid metals, the violation of the Stokes-Einstein relation signals the onset of spatially heterogeneous dynamics and collective motions. Although the viscosity of water strongly decouples from translational motion, a scaling with rotational motion remains, similar to canonical glassformers.supercooled water | viscosity | Stokes-Einstein relations W ater, considered as a potential glassformer, has been a longlasting topic of intense activity. Its possible liquid-glass transition was reported 50 years ago to be in the vicinity of 140 K (1, 2). However, ice nucleation hinders the access to this transition from the liquid side. Bypassing crystallization requires hyperquenching the liquid at tremendous cooling rates, ca. 10 7 K · s −1 (3). As a consequence, many questions about supercooled and glassy water and its glass-liquid transition remain open (4-7).As 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). 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). 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. 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). 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. Based on these and other observations, it has been hypothesized that supercooled water experiences a fragile-tostrong transition (17). This idea has motivated experimental efforts to measure dynamic properties of supercooled wate...

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“…6 (c)). Earlier studies [65][66] derived from the absorbed infrared flux [51], a density change of ~ 0.5% is expected. On a time scale of a few hundred ps after excitation, where we probe the transient x-ray absorption spectrum, the density has not changed yet.…”

Section: Resultsmentioning

confidence: 98%

Time-resolved X-ray absorption spectroscopy of infrared-laser-induced temperature jumps in liquid water

Gavrila¹,

Godehusen²,

Weniger³

et al. 2009

Appl. Phys. A

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A time-resolved x-ray absorption study of the structural dynamics of liquid water on a picosecond time scale is presented. We apply femtosecond mid-infrared pulses to resonantly excite the intramolecular O-H stretching band of liquid water and monitor the transient response in the oxygen K-edge absorption spectrum with picosecond x-ray pulses. In this way, structural changes in the hydrogen bond network of liquid water upon an ultrafast temperature jump of approximately 20 Kelvin are investigated. The changes of the x-ray absorption as induced by such a temperature jump are about 3.2 %. This demonstrates that our method serves as a sensitive probe of transient structural changes in liquid water and that combined infrared laser-synchrotron experiments with substantially shorter x-ray pulses such as generated with a femtosecond slicing scheme are possible.

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Thermal Offset Viscosities of Liquid H₂O, D₂O, and T₂O

Cited by 256 publications

References 25 publications

Communications: The fractional Stokes–Einstein equation: Application to water

Communications: The fractional Stokes–Einstein equation: Application to water

Viscosity of deeply supercooled water and its coupling to molecular diffusion

Time-resolved X-ray absorption spectroscopy of infrared-laser-induced temperature jumps in liquid water

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