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Thermodynamic Derivation of the Energy of Activation for Ice Nucleation : Volume 15, Issue 13 (03/07/2015)

By Barahona, D.

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Book Id: WPLBN0003992546
Format Type: PDF Article :
File Size: Pages 29
Reproduction Date: 2015

Title: Thermodynamic Derivation of the Energy of Activation for Ice Nucleation : Volume 15, Issue 13 (03/07/2015)  
Author: Barahona, D.
Volume: Vol. 15, Issue 13
Language: English
Subject: Science, Atmospheric, Chemistry
Collections: Periodicals: Journal and Magazine Collection, Copernicus GmbH
Publication Date:
Publisher: Copernicus Gmbh, Göttingen, Germany
Member Page: copernicus


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Barahona, D. (2015). Thermodynamic Derivation of the Energy of Activation for Ice Nucleation : Volume 15, Issue 13 (03/07/2015). Retrieved from

Description: NASA Goddard Space Flight Center, Greenbelt, MD, USA. The activation energy controls the flux of water molecules from the bulk of the liquid to the solid during the early stages of ice formation. In most studies it is estimated by direct association with the bulk properties of water, typically viscosity and self-diffusivity. As the environment in the ice–liquid interface may differ from that of the bulk this approach may introduce bias in calculated nucleation rates. In this work a phenomenological model is proposed to describe the transfer of water molecules across the ice–liquid interface. Within this framework the activation energy naturally emerges from the combination of the energy required to break hydrogen bonds in the liquid, i.e., the bulk diffusion process, and the work dissipated from the molecular rearrangement of water molecules within the ice–liquid interface. The new expression is introduced into a generalized form of classical nucleation theory. Even though no nucleation rate measurements are used to fit any of the parameters of the theory the predicted nucleation rate is in good agreement with experimental results, even at temperature as low as 190 K where it tends to be underestimated by most models. It is shown that the activation energy has a strong dependency on temperature and a weak dependency on water activity. Such dependencies are masked by thermodynamic effects at temperatures typical of homogeneous freezing of cloud droplets, however may affect the formation of ice in haze aerosol particles. The phenomenological model introduced in this work provides an independent estimation of the activation energy and the homogenous ice nucleation rate, and it may help to improve the interpretation of experimental results and the development of parameterizations for cloud formation.

Thermodynamic derivation of the energy of activation for ice nucleation

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