Topological Understanding of the Mixed Alkaline Earth Effect in Glass

Z.J. Ding, C.J. Wilkinson, J.F. Zheng, Y.N. Lin, H.S. Liu, J.X. Shen, S.H. Kim, Yuanzheng Yue, J.J. Ren, J.C. Mauro*, Q.J. Zheng*

*Corresponding author

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

The mixed alkaline earth effect (MAEE) is important for several families of industrial borosilicate and aluminosilicate glasses, including glasses used in pharmaceutical packaging and as substrates for flat panel displays. Despite the technological importance of the mixed alkaline earth effect, the physical origin of this phenomenon is not well understood, and there is currently no model to offer quantitative prediction of the effect. In this work, the MAEE is studied both experimentally and through modeling in a series of boroaluminosilicate glasses with systematic substitution of CaO with MgO. The network structure is characterized by magic angle spinning nuclear magnetic resonance (MAS NMR) analyses of 27Al, 11B, 29Si, and 23Na. Molecular dynamics (MD) simulations are conducted to simulate the glass structures and calculate the evolution of the bond angle distributions with composition. Based on the structural data, a topological constraint model is proposed to capture the MAEE on glass transition temperature (Tg), liquid fragility index (m), and Young's modulus (E) of the glasses. Results of the topological constraint model are in good quantitative agreement with experimental data. The success of the constraint model confirms that the mixed alkaline earth effect is the result of a shift in angle around oxygen in the cation-oxygen-cation bond in the glass network. This is related to the constraint strength that ultimately governs the nonlinear property variation.

Original languageEnglish
Article number119696
JournalJournal of Non-Crystalline Solids
Volume527
Number of pages9
ISSN0022-3093
DOIs
Publication statusPublished - 2019

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Earth (planet)
Glass
glass
Cations
Positive ions
Oxygen
cations
Flat panel displays
flat panel displays
Magic angle spinning
Aluminosilicates
borosilicate glass
oxygen
packaging
Drug products
glass transition temperature
metal spinning
Molecular dynamics
modulus of elasticity
Packaging

Cite this

Ding, Z. J., Wilkinson, C. J., Zheng, J. F., Lin, Y. N., Liu, H. S., Shen, J. X., ... Zheng, Q. J. (2019). Topological Understanding of the Mixed Alkaline Earth Effect in Glass. Journal of Non-Crystalline Solids, 527, [119696]. https://doi.org/10.1016/j.jnoncrysol.2019.119696
Ding, Z.J. ; Wilkinson, C.J. ; Zheng, J.F. ; Lin, Y.N. ; Liu, H.S. ; Shen, J.X. ; Kim, S.H. ; Yue, Yuanzheng ; Ren, J.J. ; Mauro, J.C. ; Zheng, Q.J. / Topological Understanding of the Mixed Alkaline Earth Effect in Glass. In: Journal of Non-Crystalline Solids. 2019 ; Vol. 527.
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abstract = "The mixed alkaline earth effect (MAEE) is important for several families of industrial borosilicate and aluminosilicate glasses, including glasses used in pharmaceutical packaging and as substrates for flat panel displays. Despite the technological importance of the mixed alkaline earth effect, the physical origin of this phenomenon is not well understood, and there is currently no model to offer quantitative prediction of the effect. In this work, the MAEE is studied both experimentally and through modeling in a series of boroaluminosilicate glasses with systematic substitution of CaO with MgO. The network structure is characterized by magic angle spinning nuclear magnetic resonance (MAS NMR) analyses of 27Al, 11B, 29Si, and 23Na. Molecular dynamics (MD) simulations are conducted to simulate the glass structures and calculate the evolution of the bond angle distributions with composition. Based on the structural data, a topological constraint model is proposed to capture the MAEE on glass transition temperature (Tg), liquid fragility index (m), and Young's modulus (E) of the glasses. Results of the topological constraint model are in good quantitative agreement with experimental data. The success of the constraint model confirms that the mixed alkaline earth effect is the result of a shift in angle around oxygen in the cation-oxygen-cation bond in the glass network. This is related to the constraint strength that ultimately governs the nonlinear property variation.",
author = "Z.J. Ding and C.J. Wilkinson and J.F. Zheng and Y.N. Lin and H.S. Liu and J.X. Shen and S.H. Kim and Yuanzheng Yue and J.J. Ren and J.C. Mauro and Q.J. Zheng",
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Ding, ZJ, Wilkinson, CJ, Zheng, JF, Lin, YN, Liu, HS, Shen, JX, Kim, SH, Yue, Y, Ren, JJ, Mauro, JC & Zheng, QJ 2019, 'Topological Understanding of the Mixed Alkaline Earth Effect in Glass', Journal of Non-Crystalline Solids, vol. 527, 119696. https://doi.org/10.1016/j.jnoncrysol.2019.119696

Topological Understanding of the Mixed Alkaline Earth Effect in Glass. / Ding, Z.J.; Wilkinson, C.J.; Zheng, J.F.; Lin, Y.N.; Liu, H.S.; Shen, J.X.; Kim, S.H.; Yue, Yuanzheng; Ren, J.J.; Mauro, J.C.; Zheng, Q.J.

In: Journal of Non-Crystalline Solids, Vol. 527, 119696, 2019.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Topological Understanding of the Mixed Alkaline Earth Effect in Glass

AU - Ding, Z.J.

AU - Wilkinson, C.J.

AU - Zheng, J.F.

AU - Lin, Y.N.

AU - Liu, H.S.

AU - Shen, J.X.

AU - Kim, S.H.

AU - Yue, Yuanzheng

AU - Ren, J.J.

AU - Mauro, J.C.

AU - Zheng, Q.J.

PY - 2019

Y1 - 2019

N2 - The mixed alkaline earth effect (MAEE) is important for several families of industrial borosilicate and aluminosilicate glasses, including glasses used in pharmaceutical packaging and as substrates for flat panel displays. Despite the technological importance of the mixed alkaline earth effect, the physical origin of this phenomenon is not well understood, and there is currently no model to offer quantitative prediction of the effect. In this work, the MAEE is studied both experimentally and through modeling in a series of boroaluminosilicate glasses with systematic substitution of CaO with MgO. The network structure is characterized by magic angle spinning nuclear magnetic resonance (MAS NMR) analyses of 27Al, 11B, 29Si, and 23Na. Molecular dynamics (MD) simulations are conducted to simulate the glass structures and calculate the evolution of the bond angle distributions with composition. Based on the structural data, a topological constraint model is proposed to capture the MAEE on glass transition temperature (Tg), liquid fragility index (m), and Young's modulus (E) of the glasses. Results of the topological constraint model are in good quantitative agreement with experimental data. The success of the constraint model confirms that the mixed alkaline earth effect is the result of a shift in angle around oxygen in the cation-oxygen-cation bond in the glass network. This is related to the constraint strength that ultimately governs the nonlinear property variation.

AB - The mixed alkaline earth effect (MAEE) is important for several families of industrial borosilicate and aluminosilicate glasses, including glasses used in pharmaceutical packaging and as substrates for flat panel displays. Despite the technological importance of the mixed alkaline earth effect, the physical origin of this phenomenon is not well understood, and there is currently no model to offer quantitative prediction of the effect. In this work, the MAEE is studied both experimentally and through modeling in a series of boroaluminosilicate glasses with systematic substitution of CaO with MgO. The network structure is characterized by magic angle spinning nuclear magnetic resonance (MAS NMR) analyses of 27Al, 11B, 29Si, and 23Na. Molecular dynamics (MD) simulations are conducted to simulate the glass structures and calculate the evolution of the bond angle distributions with composition. Based on the structural data, a topological constraint model is proposed to capture the MAEE on glass transition temperature (Tg), liquid fragility index (m), and Young's modulus (E) of the glasses. Results of the topological constraint model are in good quantitative agreement with experimental data. The success of the constraint model confirms that the mixed alkaline earth effect is the result of a shift in angle around oxygen in the cation-oxygen-cation bond in the glass network. This is related to the constraint strength that ultimately governs the nonlinear property variation.

U2 - 10.1016/j.jnoncrysol.2019.119696

DO - 10.1016/j.jnoncrysol.2019.119696

M3 - Journal article

VL - 527

JO - Journal of Non-Crystalline Solids

JF - Journal of Non-Crystalline Solids

SN - 0022-3093

M1 - 119696

ER -