Liquids at Large Negative Pressures: Water at the Homogeneous Nucleation Limit

Zheng, Qiang; Durben, Dan J.; Wolf, George H.; Angell, C. Austen

doi:10.1126/science.254.5033.829

Cited by 374 publications

(386 citation statements)

References 21 publications

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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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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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“…Pure water or aqueous solutions trapped in a solid matrix (quartz in general) were demonstrated to superheat up to very high tensions (e.g. [Green et al, 1990], [Zheng et al, 1991] and [Alvarenga et al, 1993]) with corresponding changes of phase equilibria (Roedder, 1967). The liquid tension is calculated extrapolating the equation of state (EoS) either from a micro-thermometric measurement of the homogenization and nucleation temperatures (see below) (e.g.…”

Section: Superheating Features and Previous Experimentsmentioning

confidence: 99%

“…The liquid tension is calculated extrapolating the equation of state (EoS) either from a micro-thermometric measurement of the homogenization and nucleation temperatures (see below) (e.g. [Green et al, 1990] and [Zheng et al, 1991]), or from spectroscopic (Brillouin) measurements of the speed of sound (Alvarenga et al, 1993).…”

Section: Superheating Features and Previous Experimentsmentioning

confidence: 99%

Experimental superheating of water and aqueous solutions

Shmulovich

Mercury

Thiéry

et al. 2009

Geochimica et Cosmochimica Acta

101

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The metastable superheated solutions are liquids in transitory thermodynamic equilibrium inside the stability domain of their vapor (whatever the temperature is). Some natural contexts should allow the superheating of natural aqueous solutions, like the soil capillarity (low T superheating), certain continental and submarine geysers (high T superheating), or even the water state in very arid environments like the Mars subsurface (low T) or the deep crustal rocks (high T). The present paper reports experimental measurements on the superheating range of aqueous solutions contained in quartz as fluid inclusions (Synthetic Fluid Inclusion Technique, SFIT) and brought to superheating state by isochoric cooling. About 40 samples were synthetized at 0.75 GPa and 530-700 °C with internally-heated autoclaves. Nine hundred and sixty-seven inclusions were studied by micro-thermometry, including measuring the temperatures of homogenization (Th: L + V → L) and vapor bubbles nucleation (Tn: L → L + V). The Th-Tn difference corresponds to the intensity of superheating that the trapped liquid can undergo and can be translated into liquid pressure (existing just before nucleation occurs at Tn) by an equation of state. Pure water (840-935 kg m −3 ), dilute NaOH solutions (0.1 and 0.5 mol kg −1 ), NaCl, CaCl 2 and CsCl solutions (1 and 5 mol kg −1 ) demonstrated a surprising ability to undergo tensile stress. The highest tension ever recorded to the best of our knowledge (−146 MPa, 100 °C) is attained in a 5 m CaCl 2 inclusion trapped in quartz matrix, while CsCl solutions qualitatively show still better superheating efficiency. These observations are discussed with regards to the quality of the inner surface of inclusion surfaces (high P-T synthesis conditions) and to the intrinsic cohesion of liquids (thermodynamic and kinetic spinodal). This study demonstrates that natural solutions can reach high levels of superheating, that are accompanied by strong changes of their physicochemical properties.

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“…1 This value has actually been achieved experimentally by isochoric cooling of ultraclean water in inclusions in quartz. 2 However, experimentally the tensile strength of ordinary water is found to be very low, and it is of great importance for numerous practical applications of water. Even when great care is taken in the cleaning of normal water and equipment, the highest tensile strength measured is almost an order of magnitude smaller than the theoretical one.…”

Section: Introductionmentioning

confidence: 99%

Reflections on cavitation nuclei in water

Mørch

2007

Physics of Fluids

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The origin of cavitation bubbles, cavitation nuclei, has been a subject of debate since the early years of cavitation research. This paper presents an analysis of a representative selection of experimental investigations of cavitation inception and the tensile strength of water. At atmospheric pressure, the possibility of stabilization of free gas bubbles by a skin has been documented, but only within a range of bubble sizes that makes them responsible for tensile strengths up to about 1.5 bar, and values reaching almost 300 bar have been measured. However, cavitation nuclei can also be harbored on the surface of particles and bounding walls. Such nuclei can be related to the full range of tensile strengths measured, when differences of experimental conditions are taken into consideration. The absence or presence of contamination on surfaces, as well as the structure of the surfaces, are central to explaining why the tensile strength of water varies so dramatically between the experiments reported. A model for calculation of the critical pressure of skin-covered free gas bubbles as well as that of interfacial gaseous nuclei covered by a skin is presented. This model is able to bridge the apparently conflicting results of the many scientists, who have been working in the field over the years.

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Liquids at Large Negative Pressures: Water at the Homogeneous Nucleation Limit

Cited by 374 publications

References 21 publications

Optical Kerr Effect Spectroscopy of Simple Liquids

Optical Kerr Effect Spectroscopy of Simple Liquids

Experimental superheating of water and aqueous solutions

Reflections on cavitation nuclei in water

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