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Ice is born in low-mobility regions of supercooled liquid water
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Fitzner, Martin, Sosso, Gabriele C., Cox, Stephen and Michaelides, Angelos (2019) Ice is born in low-mobility regions of supercooled liquid water. Proceedings of the National Academy of Sciences of the United States of America, 116 (6). pp. 2009-2014. doi:10.1073/pnas.1817135116 ISSN 0027-8424.
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Official URL: https://doi.org/10.1073/pnas.1817135116
Abstract
When an ice crystal is born from liquid water, two key changes occur: (i) The molecules order and (ii) the mobility of the molecules drops as they adopt their lattice positions. Most research on ice nucleation (and crystallization in general) has focused on understanding the former with less attention paid to the latter. However, supercooled water exhibits fascinating and complex dynamical behavior, most notably dynamical heterogeneity (DH), a phenomenon where spatially separated domains of relatively mobile and immobile particles coexist. Strikingly, the microscopic connection between the DH of water and the nucleation of ice has yet to be unraveled directly at the molecular level. Here we tackle this issue via computer simulations which reveal that (i) ice nucleation occurs in low-mobility regions of the liquid, (ii) there is a dynamical incubation period in which the mobility of the molecules drops before any ice-like ordering, and (iii) ice-like clusters cause arrested dynamics in surrounding water molecules. With this we establish a clear connection between dynamics and nucleation. We anticipate that our findings will pave the way for the examination of the role of dynamical heterogeneities in heterogeneous and solution-based nucleation.
Item Type: | Journal Article | ||||||||||||
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Subjects: | Q Science > QC Physics Q Science > QD Chemistry |
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||||||||||
Library of Congress Subject Headings (LCSH): | Ice nuclei, Atmospheric nucleation, Crystallization, Water of | ||||||||||||
Journal or Publication Title: | Proceedings of the National Academy of Sciences of the United States of America | ||||||||||||
Publisher: | National Academy of Sciences | ||||||||||||
ISSN: | 0027-8424 | ||||||||||||
Official Date: | 5 February 2019 | ||||||||||||
Dates: |
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Volume: | 116 | ||||||||||||
Number: | 6 | ||||||||||||
Page Range: | pp. 2009-2014 | ||||||||||||
DOI: | 10.1073/pnas.1817135116 | ||||||||||||
Status: | Peer Reviewed | ||||||||||||
Publication Status: | Published | ||||||||||||
Access rights to Published version: | Open Access (Creative Commons) | ||||||||||||
Date of first compliant deposit: | 17 January 2019 | ||||||||||||
Date of first compliant Open Access: | 26 February 2019 | ||||||||||||
RIOXX Funder/Project Grant: |
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