Water and Solutions at Negative Pressure: Raman Spectroscopic Study to -80 Megapascals

Green, J. L.; Durben, Dan J.; Wolf, George H.; Angell, C. Austen

doi:10.1126/science.249.4969.649

Cited by 121 publications

(107 citation statements)

References 21 publications

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“…The micro-thermometry technique enables to put the trapped liquid into the superheating state. Actually, the procedure ( It is interesting to notice that the sample 2 display similar (P,T) pair than that observed by Green et al 8 which was (-80 MPa; 92°C).…”

Section: Experimental Set-upmentioning

confidence: 78%

“…We are interested in this paper to deal with the following question: is the strong cohesion revealed by the superheated water a behavior of the normal -bulk‖ liquid, or is it a consequence of a special molecular networking developed under the stretching conditions? In the literature, Green et al 8 recorded the Raman spectra of an aqueous solution occluded in a fluid inclusion at 92°C, successively superheated and stable, and found the corresponding OH-stretching bands almost identical.…”

Section: Introductionmentioning

confidence: 99%

“…1), either by the Synthetic Fluid Inclusion Technique (SFIT hereafter) [8][9][10][11] , or by other techniques (see a recent review in Ref. 12).…”

Section: Introductionmentioning

confidence: 99%

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Infra-red imaging of bulk water and water–solid interfaces under stable and metastable conditions

Mercury¹,

Jamme²,

Dumas³

2012

Phys. Chem. Chem. Phys.

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To cite this version:Lionel Mercury, Frédéric Jamme, Paul Dumas. Infra-red imaging of bulk water and water-solid interfaces under stable and metastable conditions.. Physical Chemistry Chemical Physics, Royal Society of Chemistry, 2012Chemistry, , 14, pp.2864Chemistry, -2874.1039/C2CP23221A>. AbstractSuperheated water has been studied by infrared spectroscopy to examine whether the special ability of liquid water to undergo such metastable state corresponds to the development of peculiar inter-molecular networking under tension. As the best technique to superheat water is to trap the liquid inside micro-cavities in solids (the so-called -fluid inclusions‖), the role of the water-solid interfaces to stabilize the adjoining liquid is also explored with the same infra-red micro-spectroscopy tool. The key signal is the intramolecular OH stretching band, sensitive to the networking in the probed material. The sample of choice is liquid water occluded inside quartz cavity of micrometric size, synthetized in laboratory from pure quartz and milli-Q water. The stretching band of the superheated water shows no significant spectral difference with that of a bulk -normal‖ water, which means that the molecular properties of the superheating liquid is quite similar to those of the stable bulk liquid. Liquid water is readily -superheatable‖ but retains its -normality‖ under these special conditions. Additionally, this result establishes a firm ground to justify that the properties of the former are predicted extrapolating the usual (though empirical) equation of state of the latter. The infra-red signals of the water-solid interfaces are more complex. The water-solid interfaces blue-shift the signal, affecting differently the three sub-bands of the OH-stretching. This effect was unexpected since the micro-IR spectroscopy probes volume beyond of what is classicaly assigned for the interfacial properties. In addition, the interfacial signature is clearer under superheating than with the saturation conditions, which offers an interesting (and unexpected) way to interpret the special stability of the occluded metastable water. These encouraging results give confidence on the potentialities of the high-resolution micro-spectroscopy to get insights into the molecular basis of macroscopic properties.

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Section: Experimental Set-upmentioning

confidence: 78%

Section: Introductionmentioning

confidence: 99%

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Infra-red imaging of bulk water and water–solid interfaces under stable and metastable conditions

Mercury¹,

Jamme²,

Dumas³

2012

Phys. Chem. Chem. Phys.

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“…[57][58][59][60][61][62][63][64] Water is in many ways an ideal liquid for such studies, in that it has an extremely high tensile strength for a liquid due to the high degree of hydrogen bonding. However, heterogeneous nucleation generally prevents water from being stretched to its intrinsic tensile strength.…”

Section: T 1 T Fill T 2 > T Fill T 3 < T Fill T Break < Tmentioning

confidence: 99%

Optical Kerr Effect Spectroscopy of Simple Liquids

2008

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Optical Kerr effect (OKE) spectroscopy has become a prominent nonlinear optical technique for studying liquids, which allows for the direct, time-resolved probing of collective orientational diffusion as well as Raman-active intermolecular and intramolecular modes.The temperature-dependent orientational dynamics of 1, n-dicyano n-alkane liquids ranging from dicyanomethane to 1,8-dicyanooctane has been investigated by ultrafast OKE spectroscopy. The dependence of the reorientational times on temperature and viscosity is consistent with the molecules adopting a largely extended structure in the liquid state, with a preference for gauche conformations at the methylenes bonded to the cyanide groups. The data are also suggestive of temperature-dependent, collective structural rearrangements in these liquids.Ultrafast OKE spectroscopy has also been used to study the intermolecular dynamics of aromatic liquids. A model that links the differences in the OKE spectra to corresponding differences in the local ordering of the liquids has been proposed previously based on the temperature-dependent OKE study of five aromatic liquids.The spectra of some other aromatic liquids such as pyridine, pyridine-d5, 2,4,6-trifluoropyridine and 1,3,5-tris(trifluoromethyl) benzene has been obtained to test this model, and the relative importance of molecular shape and electrostatic forces in determining the form of the OKE reduced spectral density for such liquids has been realized. It has recently been shown that liquid tetrahydrofuran (THF) has an unusual structure that features voids of significant dimension. Such voids should affect other observable properties of this liquid. Temperature-dependent, optical Kerr effect spectra for THF and a number of related liquids (furan, cyclopentane, tetrahydropyran, cyclohexane, diethyl ether, hexamethylphosphoramide and n-pentane) has been obtained to test whether the shape of the spectra can be used to reveal the presence of sizeable voids in liquids. Liquid under tension is another interesting system to study:A method based on Berthelot tube technique has been developed to hold benzene and acetonitrile under tension successfully.A new scheme for measuring different tensor elements of the OKE response is developed. A dual-ring, polarization dependent Sagnac interferometer is used to create two co-propagating probe pulses that arrive at the sample at different times but that reach the detector simultaneously and collinearly. The tensor element of the response that is measured is determined by the polarization of the pump pulse. By controlling the relative timing of the probe pulses it is also possible to perform optical subtraction of two different tensor elements of the response at two different times, a strategy that can be used to enhance or suppress particular contributions to the OKE response. OPTICAL KERR EFFECT SPECTROSCOPY OF SIMPLE LIQUIDS

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“…Analytical work on simple potentials showing a density maximum should also be pursued; already such approaches have revealed a rich set of possible behaviors [16][17][18][19][20][34][35][36][37] ]. If our data are confirmed by these extensive checks, then it will become important to perform experiments as close as possible to the new critical point, which according to the P and T shift used above, should be located in real water at T = 185 K and P = 120 Pa. At the same time, we hope that measurements in the stretched region can be extended to search for the change in slope of the line of density maxima [38 ].…”

Section: A New Critical Point?mentioning

confidence: 99%

Is there a second critical point in liquid water?

Stanley

Angell

Essmann

et al. 1994

Physica A: Statistical Mechanics and its Applications

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The supercooled and stretched regions of the phase diagram of simulated liquid water are investigated by calculating the equation of state of the ST2 and TIP4P pair-potentials. We find that simulated water does not display a re-entrant spinodal and that the projection of the density maximum line in the plane of pressure and temperature becomes positively sloped on stretching. The well-known anomalous behavior of supercooled water is tentatively associated with the existence of an inaccessible critical point. Evidence is presented that suggests the association of this new critical point with the transition between low density and high density amorphous solid water. We show how the observed transformation behavior of the two forms of amorphous solid water can be explained in terms of a first order phase transition, via a consideration of the limits of metastability associated with this kind of transition, and support this interpretation with simulations of the amorphous solid. We therefore propose a phase diagram which accounts for the behavior of both liquid and amorphous solid water.

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Water and Solutions at Negative Pressure: Raman Spectroscopic Study to -80 Megapascals

Cited by 121 publications

References 21 publications

Infra-red imaging of bulk water and water–solid interfaces under stable and metastable conditions

Infra-red imaging of bulk water and water–solid interfaces under stable and metastable conditions

Optical Kerr Effect Spectroscopy of Simple Liquids

Is there a second critical point in liquid water?

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