Detecting vapour bubbles in simulations of metastable water

International audienceThe investigation of cavitation in metastable liquids with molecular simulations requires an appropriate definition of the volume of the vapour bubble forming within the metastable liquid phase. Commonly used approaches for bubble detection exhibit two significant flaws: first, when applied to water they often identify the voids within the hydrogen bond network as bubbles thus masking the signature of emerging bubbles and, second, they lack thermodynamic consistency. Here, we present two grid-based methods, the M-method and the V-method, to detect bubbles in metastable water specifically designed to address these shortcomings. The M-method incorporates information about neighbouring grid cells to distinguish between liquid- and vapour-like cells, which allows for a very sensitive detection of small bubbles and high spatial resolution of the detected bubbles. The V-method is calibrated such that its estimates for the bubble volume correspond to the average change in system volume and are thus thermodynamically consistent. Both methods are computationally inexpensive such that they can be used in molecular dynamics and Monte Carlo simulations of cavitation. We illustrate them by computing the free energy barrier and the size of the critical bubble for cavitation in water at negative pressure

Cavitation pressure in liquid helium

Recent experiments have suggested that, at low enough temperature, the homogeneous nucleation of bubbles occurs in liquid helium near the calculated spinodal limit. This was done in pure superfluid helium 4 and in pure normal liquid helium 3. However, in such experiments, where the negative pressure is produced by focusing an acoustic wave in the bulk liquid, the local amplitude of the instantaneous pressure or density is not directly measurable. In this article, we present a series of measurements as a function of the static pressure in the experimental cell. They allowed us to obtain an upper bound for the cavitation pressure P_cav (at low temperature, P_cav < -2.4 bar in helium 3, P_cav < -8.0 bar in helium 4). From a more precise study of the acoustic transducer characteristics, we also obtained a lower bound (at low temperature, P_cav > -3.0 bar in helium 3, P_cav > - 10.4 bar in helium 4). In this article we thus present quantitative evidence that cavitation occurs at low temperature near the calculated spinodal limit (-3.1 bar in helium 3 and -9.5 bar in helium 4). Further information is also obtained on the comparison between the two helium isotopes. We finally discuss the magnitude of nonlinear effects in the focusing of a sound wave in liquid helium, where the pressure dependence of the compressibility is large.Comment: 11 pages, 9 figure

Anomaly in the stability limit of liquid helium 3

We propose that the liquid-gas spinodal line of helium 3 reaches a minimum at 0.4 K. This feature is supported by our cavitation measurements. We also show that it is consistent with extrapolations of sound velocity measurements. Speedy [J. Phys. Chem. 86, 3002 (1982)] previously proposed this peculiar behavior for the spinodal of water and related it to a change in sign of the expansion coefficient alpha, i. e. a line of density maxima. Helium 3 exhibits such a line at positive pressure. We consider its extrapolation to negative pressure. Our discussion raises fundamental questions about the sign of alpha in a Fermi liquid along its spinodal.Comment: 5 pages, 3 figure

Quantum cavitation in liquid 3^3He: dissipation effects

We have investigated the effect that dissipation may have on the cavitation process in normal liquid $^3$He. Our results indicate that a rather small dissipation decreases sizeably the quantum-to-thermal crossover temperature $T^*$ for cavitation in normal liquid $^3$He. This is a possible explanation why recent experiments have not yet found clear evidence of quantum cavitation at temperatures below the $T^*$ predicted by calculations which neglect dissipation.Comment: To be published in Physical Review B6

The shock compression of microorganism-loaded broths and emulsions: Experiments and simulations

By carefully selecting flyer plate thickness and the geometry of a target capsule for bacterial broths and emulsions, we have successfully subjected the contents of the capsule to simultaneous shock and dynamic compression when subjected to a flyer-plate impact experiment. The capsules were designed to be recovered intact so that post experimental analysis could be done on the contents. ANSYS® AUTODYN hydrocode simulations were carried out to interrogate the deformation of the cover plate and the wave propagation in the fluid. Accordingly, we have shown that microorganisms such as Escherichia coli, Enterococcus faecalis and Zygosaccharomyces bailii are not affected by this type of loading regime. However, by introducing a cavity behind the broth we were able to observe limited kill in the yeast sample. Further, on using this latter technique with emulsions it was shown that greater emulsification of an oil-based emulsion occurred due to the cavitation that was introduced

Critical Casimir effect and wetting by helium mixtures

We have measured the contact angle of the interface of phase-separated $^{3}$He-$^{4}$He mixtures against a sapphire window. We have found that this angle is finite and does not tend to zero when the temperature approaches $T_t$, the temperature of the tri-critical point. On the contrary, it increases with temperature. This behavior is a remarkable exception to what is generally observed near critical points, i.e. "critical point wetting''. We propose that it is a consequence of the "critical Casimir effect'' which leads to an effective attraction of the $^{3}$He-$^{4}$He interface by the sapphire near $T_{t}$.Comment: submitted july 13 (2002), published march 20 (2003

Homogeneous Bubble Nucleation driven by local hot spots: a Molecular Dynamics Study

We report a Molecular Dynamics study of homogenous bubble nucleation in a Lennard-Jones fluid. The rate of bubble nucleation is estimated using forward-flux sampling (FFS). We find that cavitation starts with compact bubbles rather than with ramified structures as had been suggested by Shen and Debenedetti (J. Chem. Phys. 111:3581, 1999). Our estimate of the bubble-nucleation rate is higher than predicted on the basis of Classical Nucleation Theory (CNT). Our simulations show that local temperature fluctuations correlate strongly with subsequent bubble formation - this mechanism is not taken into account in CNT

Toward a Density Functional Description of Liquid pH(2)

A finite-temperature density functional approach to describe the properties of parahydrogen in the liquid-vapor coexistence region is presented. The first proposed functional is zero-range, where the density-gradient term is adjusted so as to reproduce the surface tension of the liquid-vapor interface at low temperature. The second functional is finite-range and, while it is fitted to reproduce bulk pH(2) properties only, it is shown to yield surface properties in good agreement with experiments. These functionals are used to study the surface thickness of the liquid-vapor interface, the wetting transition of parahydrogen on a planar Rb model surface, and homogeneous cavitation in bulk liquid pH(2)