Modifier clustering and avoidance principle in borosilicate glasses: A molecular dynamics study

Mengyi Wang, Morten M. Smedskjaer, John Mauro, Mathieu Bauchy

Research output: Contribution to journalArticle

Abstract

Oxide glasses are typically described as having a random, disordered skeleton of network-forming polyhedra that are depolymerized by network-modifying cations. However, the existence of local heterogeneity or clustering within the network-forming and network-modifying species remains unclear. Here, based on molecular dynamics simulations, we investigate the atomic structure of a series of borosilicate glasses. We show that the network-modifying cations exhibit some level of clustering that depends on composition - in agreement with Greaves' modified random network model. In addition, we demonstrate the existence of some mutual avoidance among network-forming atoms, which echoes the Loewenstein avoidance principle typically observed in aluminosilicate phases. Importantly, we demonstrate that the degree of heterogeneity in the spatial distribution of the network modifiers is controlled by the level of ordering in the interconnectivity of the network formers. Specifically, the mutual avoidance of network formers is found to decrease the propensity for modifier clustering.

Original languageEnglish (US)
Article number044502
JournalJournal of Chemical Physics
Volume150
Issue number4
DOIs
StatePublished - Jan 28 2019

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Borosilicate glass
avoidance
borosilicate glass
Molecular dynamics
Cations
molecular dynamics
Oxides
Spatial distribution
Glass
Atoms
Computer simulation
Chemical analysis
cations
polyhedrons
musculoskeletal system
atomic structure
echoes
spatial distribution
aluminosilicate

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

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abstract = "Oxide glasses are typically described as having a random, disordered skeleton of network-forming polyhedra that are depolymerized by network-modifying cations. However, the existence of local heterogeneity or clustering within the network-forming and network-modifying species remains unclear. Here, based on molecular dynamics simulations, we investigate the atomic structure of a series of borosilicate glasses. We show that the network-modifying cations exhibit some level of clustering that depends on composition - in agreement with Greaves' modified random network model. In addition, we demonstrate the existence of some mutual avoidance among network-forming atoms, which echoes the Loewenstein avoidance principle typically observed in aluminosilicate phases. Importantly, we demonstrate that the degree of heterogeneity in the spatial distribution of the network modifiers is controlled by the level of ordering in the interconnectivity of the network formers. Specifically, the mutual avoidance of network formers is found to decrease the propensity for modifier clustering.",
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Modifier clustering and avoidance principle in borosilicate glasses : A molecular dynamics study. / Wang, Mengyi; Smedskjaer, Morten M.; Mauro, John; Bauchy, Mathieu.

In: Journal of Chemical Physics, Vol. 150, No. 4, 044502, 28.01.2019.

Research output: Contribution to journalArticle

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T1 - Modifier clustering and avoidance principle in borosilicate glasses

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AU - Wang, Mengyi

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