The role of structural order in heterogeneous ice nucleation

The freezing of water into ice is a key process that is still not fully understood. It generally requires an impurity of some description to initiate the heterogeneous nucleation of the ice crystals. The molecular structure, as well as the extent of structural order within the impurity in question,...

Descripción completa

Detalles Bibliográficos
Autores principales: Sosso, Gabriele C., Sudera, Prerna, Backes, Anna T., Whale, Thomas F., Fröhlich-Nowoisky, Janine, Bonn, Mischa, Michaelides, Angelos, Backus, Ellen H. G.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9067566/
https://www.ncbi.nlm.nih.gov/pubmed/35655890
http://dx.doi.org/10.1039/d1sc06338c
_version_ 1784700033544749056
author Sosso, Gabriele C.
Sudera, Prerna
Backes, Anna T.
Whale, Thomas F.
Fröhlich-Nowoisky, Janine
Bonn, Mischa
Michaelides, Angelos
Backus, Ellen H. G.
author_facet Sosso, Gabriele C.
Sudera, Prerna
Backes, Anna T.
Whale, Thomas F.
Fröhlich-Nowoisky, Janine
Bonn, Mischa
Michaelides, Angelos
Backus, Ellen H. G.
author_sort Sosso, Gabriele C.
collection PubMed
description The freezing of water into ice is a key process that is still not fully understood. It generally requires an impurity of some description to initiate the heterogeneous nucleation of the ice crystals. The molecular structure, as well as the extent of structural order within the impurity in question, both play an essential role in determining its effectiveness. However, disentangling these two contributions is a challenge for both experiments and simulations. In this work, we have systematically investigated the ice-nucleating ability of the very same compound, cholesterol, from the crystalline (and thus ordered) form to disordered self-assembled monolayers. Leveraging a combination of experiments and simulations, we identify a “sweet spot” in terms of the surface coverage of the monolayers, whereby cholesterol maximises its ability to nucleate ice (which remains inferior to that of crystalline cholesterol) by enhancing the structural order of the interfacial water molecules. These findings have practical implications for the rational design of synthetic ice-nucleating agents.
format Online
Article
Text
id pubmed-9067566
institution National Center for Biotechnology Information
language English
publishDate 2022
publisher The Royal Society of Chemistry
record_format MEDLINE/PubMed
spelling pubmed-90675662022-06-01 The role of structural order in heterogeneous ice nucleation Sosso, Gabriele C. Sudera, Prerna Backes, Anna T. Whale, Thomas F. Fröhlich-Nowoisky, Janine Bonn, Mischa Michaelides, Angelos Backus, Ellen H. G. Chem Sci Chemistry The freezing of water into ice is a key process that is still not fully understood. It generally requires an impurity of some description to initiate the heterogeneous nucleation of the ice crystals. The molecular structure, as well as the extent of structural order within the impurity in question, both play an essential role in determining its effectiveness. However, disentangling these two contributions is a challenge for both experiments and simulations. In this work, we have systematically investigated the ice-nucleating ability of the very same compound, cholesterol, from the crystalline (and thus ordered) form to disordered self-assembled monolayers. Leveraging a combination of experiments and simulations, we identify a “sweet spot” in terms of the surface coverage of the monolayers, whereby cholesterol maximises its ability to nucleate ice (which remains inferior to that of crystalline cholesterol) by enhancing the structural order of the interfacial water molecules. These findings have practical implications for the rational design of synthetic ice-nucleating agents. The Royal Society of Chemistry 2022-04-08 /pmc/articles/PMC9067566/ /pubmed/35655890 http://dx.doi.org/10.1039/d1sc06338c Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by/3.0/
spellingShingle Chemistry
Sosso, Gabriele C.
Sudera, Prerna
Backes, Anna T.
Whale, Thomas F.
Fröhlich-Nowoisky, Janine
Bonn, Mischa
Michaelides, Angelos
Backus, Ellen H. G.
The role of structural order in heterogeneous ice nucleation
title The role of structural order in heterogeneous ice nucleation
title_full The role of structural order in heterogeneous ice nucleation
title_fullStr The role of structural order in heterogeneous ice nucleation
title_full_unstemmed The role of structural order in heterogeneous ice nucleation
title_short The role of structural order in heterogeneous ice nucleation
title_sort role of structural order in heterogeneous ice nucleation
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9067566/
https://www.ncbi.nlm.nih.gov/pubmed/35655890
http://dx.doi.org/10.1039/d1sc06338c
work_keys_str_mv AT sossogabrielec theroleofstructuralorderinheterogeneousicenucleation
AT suderaprerna theroleofstructuralorderinheterogeneousicenucleation
AT backesannat theroleofstructuralorderinheterogeneousicenucleation
AT whalethomasf theroleofstructuralorderinheterogeneousicenucleation
AT frohlichnowoiskyjanine theroleofstructuralorderinheterogeneousicenucleation
AT bonnmischa theroleofstructuralorderinheterogeneousicenucleation
AT michaelidesangelos theroleofstructuralorderinheterogeneousicenucleation
AT backusellenhg theroleofstructuralorderinheterogeneousicenucleation
AT sossogabrielec roleofstructuralorderinheterogeneousicenucleation
AT suderaprerna roleofstructuralorderinheterogeneousicenucleation
AT backesannat roleofstructuralorderinheterogeneousicenucleation
AT whalethomasf roleofstructuralorderinheterogeneousicenucleation
AT frohlichnowoiskyjanine roleofstructuralorderinheterogeneousicenucleation
AT bonnmischa roleofstructuralorderinheterogeneousicenucleation
AT michaelidesangelos roleofstructuralorderinheterogeneousicenucleation
AT backusellenhg roleofstructuralorderinheterogeneousicenucleation