Modeling Oxygen Tricluster Formation in Calcium Aluminosilicate Supercooled Liquids and Glasses

Calcium aluminosilicate glasses have technological importance for a variety of industrial applications. However, the short-range structure of this glass system remains widely debated regarding the formation of oxygen triclusters. It is argued that triclusters are observed in high percentages within...

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Bibliographic Details
Published in:	The journal of physical chemistry. B Vol. 126; no. 40; pp. 8039 - 8047
Main Authors:	Astle, Sierra R., Welch, Rebecca S., Wilkinson, Collin J., Bødker, Mikkel L., Kirchner, Katelyn A., Smedskjaer, Morten M., Mauro, John C.
Format:	Journal Article
Language:	English
Published:	American Chemical Society 13-10-2022
Subjects:	B: Soft Matter, Fluid Interfaces, Colloids, Polymers, and Glassy Materials
Online Access:	Get full text
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Summary:	Calcium aluminosilicate glasses have technological importance for a variety of industrial applications. However, the short-range structure of this glass system remains widely debated regarding the formation of oxygen triclusters. It is argued that triclusters are observed in high percentages within molecular dynamics simulations because of the high melting temperatures and correspondingly high fictive temperatures. This work explores the formation of such structural units by first simulating various compositions at different liquid temperatures to understand thermodynamic factors affecting the formation of such species. Structural results are then implemented into a statistical mechanical model which can predict the formation of triclusters at a given fictive temperature. Results show temperature and composition dependence of these structures, with aluminum charge modification favored in the peraluminous regime. It is concluded that oxygen triclusters are the preferred method of charge compensation even when extrapolating to laboratory fictive temperatures, indicating that triclusters are not a byproduct of simulation timescales.
Bibliography:	ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23
ISSN:	1520-6106 1520-5207
DOI:	10.1021/acs.jpcb.2c03949