Vincent Holten

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A comparison is made between two models of homogeneous nucleation and droplet growth. The first is a kinetic model yielding the master equations for the concentrations of molecular clusters. Such a model does not make an explicit distinction between nucleation and droplet growth. The second model treats nucleation and growth separately, fully ignoring(More)
Twenty years ago Poole et al. suggested that the anomalous properties of supercooled water may be caused by a critical point that terminates a line of liquid-liquid separation of lower-density and higher-density water. Here we present a thermodynamic model based on this hypothesis, which describes all available experimental data for supercooled water with(More)
We review the available experimental information on the thermodynamic properties of supercooled water and demonstrate the possibility of modeling these thermodynamic properties on a theoretical basis. We show that by assuming the existence of a liquid-liquid critical point in supercooled water, the theory of critical phenomena can give an accurate account(More)
The thermodynamic properties of the supercooled liquid state of the mW model of water show anomalous behavior. Like in real water, the heat capacity and compressibility sharply increase upon supercooling. One of the possible explanations of these anomalies, the existence of a second (liquid-liquid) critical point, is not supported by simulations for this(More)
A popular hypothesis that explains the anomalies of supercooled water is the existence of a metastable liquid-liquid transition hidden below the line of homogeneous nucleation. If this transition exists and if it is terminated by a critical point, the addition of a solute should generate a line of liquid-liquid critical points emanating from the critical(More)
Thermodynamic properties of the ST2 model for supercooled liquid water exhibit anomalies similar to those observed in real water. A possible explanation of these anomalies is the existence of a metastable, liquid-liquid transition terminated by a critical point. This phenomenon, whose possible existence in real water is the subject of much current(More)
The heat capacity of supercooled water, measured down to -37°C, shows an anomalous increase as temperature decreases. The thermal diffusivity, i.e., the ratio of the thermal conductivity and the heat capacity per unit volume, shows a decrease. These anomalies may be associated with a hypothesized liquid-liquid critical point in supercooled water below the(More)
We have measured homogeneous nucleation rates of water at 200-240 K in the carrier gas helium, in the range of 10(13) - 10(17) m(-3) s(-1) using an expansion wave tube. The rates agree well with the results of Wolk and Strey [J. Phys. Chem. B 105, 11683 (2001)] in the range of overlap (220-240 K), and are summarized by the empirical fit J = S exp[4.6 +(More)
Homogeneous nucleation rates and droplet growth rates of water in pure methane and mixtures of methane and carbon dioxide were measured in an expansion wave tube at 235 K and 10 bar. The nucleation rate in pure methane is three orders of magnitude higher than literature nucleation rates of water in low-pressure helium or argon. Addition of carbon dioxide to(More)
Water keeps puzzling scientists because of its numerous properties which behave oppositely to those of usual liquids: for instance, water expands upon cooling, and liquid water is denser than ice. To explain this anomalous behavior, several theories have been proposed, with different predictions for the properties of supercooled water (liquid at conditions(More)