Minimum in the pressure dependence of the interfacial free energy between ice Ih and water

Author(s)
P. Montero De Hijes, J. R Espinosa, C. Vega, C. Dellago
Abstract

Despite the importance of ice nucleation, this process has been barely explored at negative pressures. Here, we study homogeneous ice nucleation in stretched water by means of molecular dynamics seeding simulations using the TIP4P/Ice model. We observe that the critical nucleus size, interfacial free energy, free energy barrier, and nucleation rate barely change between isobars from -2600 to 500 bars when they are represented as a function of supercooling. This allows us to identify universal empirical expressions for homogeneous ice nucleation in the pressure range from -2600 to 500 bars. We show that this universal behavior arises from the pressure dependence of the interfacial free energy, which we compute by means of the mold integration technique, finding a shallow minimum around -2000 bars. Likewise, we show that the change in the interfacial free energy with pressure is proportional to the excess entropy and the slope of the melting line, exhibiting in the latter a reentrant behavior also at the same negative pressure. Finally, we estimate the excess internal energy and the excess entropy of the ice Ih-water interface.

Organisation(s)
Computational and Soft Matter Physics
External organisation(s)
Universidad Complutense de Madrid
Journal
Journal of Chemical Physics
Volume
158
No. of pages
10
ISSN
0021-9606
DOI
https://doi.org/10.1063/5.0140814
Publication date
03-2023
Peer reviewed
Yes
Austrian Fields of Science 2012
103015 Condensed matter, 103006 Chemical physics
ASJC Scopus subject areas
General Physics and Astronomy, Physical and Theoretical Chemistry
Portal url
https://ucrisportal.univie.ac.at/en/publications/19bfd192-2ffa-4f3b-b87b-51d81bc112b6