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Unravelling the origins of ice nucleation on organic crystals

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Sosso, Gabriele C., Whale, Thomas Francis, Holden, Mark Andrew, Pedevilla, Philipp, Murray, Benjamin John and Michaelides, Angelos (2018) Unravelling the origins of ice nucleation on organic crystals. Chemical Science . doi:10.1039/C8SC02753F (In Press)

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Official URL: http://dx.doi.org/10.1039/C8SC02753F

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Abstract

Organic molecules such as steroids or amino acids form crystals that can facilitate the formation of ice - arguably the most important phase transition on earth. However, the origin of the ice nucleating ability of organic crystals is still largely unknown. Here, we combine experiments and simulations to unravel the microscopic details of ice formation on cholesterol, a prototypical organic crystal widely used in cryopreservation. We find that cholesterol - which is also a substantial component of cell membranes - is an ice nucleating agent more potent than many inorganic substrates, including the mineral feldspar (one of the most active ice nucleating material in the atmosphere). Scanning electron microscopy measurements reveal a variety of morphological features on the surfaces of cholesterol crystals: this suggests that the topography of the surface is key to the broad range of ice nucleating activity observed (from -4 to -20 Co). In addition, we show via molecular simulations that cholesterol crystals aid the formation of ice nuclei in a unconventional fashion. Rather than providing a template for a flat ice-like contact layer (as found in the case of many inorganic substrates), the flexibility of the cholesterol surface and its low density of hydrophilic functional groups leads to the formation of molecular cages involving both water molecules and terminal hydroxyl groups of the cholesterol surface. These cages are made of 6- and, surprisingly, 5-membered hydrogen bonded rings of water and hydroxyl groups that favour the nucleation of hexagonal as well as cubic ice (a rare occurrence). We argue that the phenomenal ice nucleating activity of steroids such as cholesterol (and potentially of many other organic crystals) is due to (i) the ability of flexible hydrophilic surfaces to form unconventional ice-templating structures and (ii) the different nucleation sites offered by the diverse topography of the crystalline surfaces. These findings clarify how exactly organic crystals promote the formation of ice, thus paving the way toward the understanding of ice formation in soft and biological matter - with obvious reverberations on atmospheric science and cryobiology.

Item Type: Journal Article
Subjects: Q Science > QH Natural history > QH301 Biology
Q Science > QP Physiology
Divisions: Faculty of Science > Chemistry
Library of Congress Subject Headings (LCSH): Cells -- Cryopreservation, Cryobiology, Cholesterol
Journal or Publication Title: Chemical Science
Publisher: Royal Society of Chemistry
ISSN: 2041-6520
Official Date: 27 August 2018
Dates:
DateEvent
27 August 2018Available
27 August 2018Accepted
Date of first compliant deposit: 29 August 2018
DOI: 10.1039/C8SC02753F
Status: Peer Reviewed
Publication Status: In Press
Access rights to Published version: Open Access
RIOXX Funder/Project Grant:
Project/Grant IDRIOXX Funder NameFunder ID
616121 (HeteroIce project)Seventh Framework Programmehttp://dx.doi.org/10.13039/100011102
632272 (IceControl project)Seventh Framework Programmehttp://dx.doi.org/10.13039/100011102
648661 (MarineIce project)Seventh Framework Programmehttp://dx.doi.org/10.13039/100011102
EP/M003027/1[EPSRC] Engineering and Physical Sciences Research Councilhttp://dx.doi.org/10.13039/501100000266
EP/L000202[EPSRC] Engineering and Physical Sciences Research Councilhttp://dx.doi.org/10.13039/501100000266
ID s758Swiss National Supercomputing Centre (CSCS)UNSPECIFIED

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