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  4. Theoretical prediction of the homogeneous ice nucleation rate: disentangling thermodynamics and kinetics
 
research article

Theoretical prediction of the homogeneous ice nucleation rate: disentangling thermodynamics and kinetics

Cheng, Bingqing  
•
Dellago, Christoph
•
Ceriotti, Michele  
December 7, 2018
Physical Chemistry Chemical Physics

Estimating the homogeneous ice nucleation rate from undercooled liquid water is crucial for understanding many important physical phenomena and technological applications, and challenging for both experiments and theory. From a theoretical point of view, difficulties arise due to the long time scales required, as well as the numerous nucleation pathways involved to form ice nuclei with different stacking disorders. We computed the homogeneous ice nucleation rate at a physically relevant undercooling for a single-site water model, taking into account the diffuse nature of ice-water interfaces, stacking disorders in ice nuclei, and the addition rate of particles to the critical nucleus. We disentangled and investigated the relative importance of all the terms, including interfacial free energy, entropic contributions and the kinetic prefactor, that contribute to the overall nucleation rate. Breaking down the problem into pieces not only provides physical insights into ice nucleation, but also sheds light on the long-standing discrepancy between different theoretical predictions, as well as between theoretical and experimental determinations of the nucleation rate. Moreover, we pinpoint the main shortcomings and suggest strategies to systematically improve the existing simulation methods.

  • Details
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Type
research article
DOI
10.1039/c8cp04561e
Web of Science ID

WOS:000451089900035

Author(s)
Cheng, Bingqing  
Dellago, Christoph
Ceriotti, Michele  
Date Issued

2018-12-07

Published in
Physical Chemistry Chemical Physics
Volume

20

Issue

45

Start page

28732

End page

28740

Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

interfacial free-energy

•

molecular-dynamics

•

crystal-nucleation

•

water

•

simulations

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
FunderGrant Number

FNS

200021-159896 NQE

Available on Infoscience
December 13, 2018
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/152038
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