Homogeneous water nucleation in a laminar flow diffusion chamber

Manka, Alexandra A.; Brus, David; Hyvärinen, Antti-Pekka; Lihavainen, Heikki; Wölk, Judith; Strey, Reinhard

doi:doi:10.1063/1.3427537

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Ice crystallization in water’s “no-man’s land”

The crystallization of water at 180 K is studied through large-scale molecular dynamics simulations with the monatomic water model mW. This temperature is in the middle of water’s “no-man’s land,” where rapid ice crystallization prevents the elucidation of the structure of liquid water and its transformation into ice with state of the art experimental methods. We find that critical ice nuclei (that contain less than ten water molecules) form in a time scale shorter than the time required for th...

Escape of a driven particle from a metastable state: A semiclassical approach

In this article we explore the dynamics of escape of a particle in the semiclassical regime by driving the particle externally. We demonstrate that under suitable approximations the semiclassical escape rate essentially assumes the structure of classical Kramers rate. Both internal (due to thermal bath) as well as external noises (due to driving) are being considered. The noises are stationary, Gaussian, and are characterized by arbitrary decaying memory kernel. Finally, we subject our formulat...

Homogeneous nucleation rates of water at temperatures between 240 and 270 K were measured in a laminar flow diffusion chamber at ambient pressure and helium as carrier gas. Being in the range of 10²–10⁶ cm⁻³ s⁻¹, the experimental results extend the nucleation rate data from literature consistently and fill a pre-existing gap. Using the macroscopic vapor pressure, density, and surface tension for water we calculate the nucleation rates predicted by classic nucleation theory (CNT) and by the empirical correction function of CNT by Wölk and Strey [J. Phys. Chem. B 105, 11683 (2001)] . As in the case of other systems (e.g., alcohols), CNT predicts a stronger temperature dependence than experimentally observed, whereas the agreement with the empirical correction function is good for all data sets. Furthermore, the isothermal nucleation rate curves allow us to determine the experimental critical cluster sizes by use of the nucleation theorem. A comparison with the critical cluster sizes calculated by use of the Gibbs–Thomson equation is remarkably good for small cluster sizes, for bigger ones the Gibbs–Thomson equation overestimates the cluster sizes.

Article Outline

INTRODUCTION
EXPERIMENT
1. Principle of operation
2. Experimental procedure
3. Data analysis
RESULTS AND DISCUSSION
1. Nucleation rates
2. Critical cluster sizes
CONCLUSION

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KEYWORDS and PACS

Keywords

density, laminar flow, nucleation, surface tension, vapour pressure

PACS

64.60.qj

Studies of nucleation in specific substances
68.03.Cd

Surface tension and related phenomena
47.15.-x

Laminar flows

ARTICLE DATA

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http://dx.doi.org/10.1063/1.3427537

PUBLICATION DATA

ISSN

0021-9606 (print)

1089-7690 (online)

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$abstract.society.value is a Member of CrossRef

American Institute of Physics

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