TY - JOUR
T1 - Modeling Oxygen Tricluster Formation in Calcium Aluminosilicate Supercooled Liquids and Glasses
AU - Astle, Sierra R.
AU - Welch, Rebecca S.
AU - Wilkinson, Collin J.
AU - Bødker, Mikkel Sandfeld
AU - Kirchner, Katelyn A.
AU - Smedskjær, Morten Mattrup
AU - Mauro, John C.
PY - 2022/10/3
Y1 - 2022/10/3
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85139699295&partnerID=8YFLogxK
U2 - 10.1021/acs.jpcb.2c03949
DO - 10.1021/acs.jpcb.2c03949
M3 - Journal article
SN - 1520-6106
VL - 126
SP - 8039
EP - 8047
JO - Journal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical
JF - Journal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical
IS - 40
ER -