Revealing the relationship between liquid fragility and medium-range order in silicate glasses

Shi, Ying; Deng, Binghui; Gulbiten, Ozgur; Bauchy, Mathieu; Zhou, Qi; Neuefeind, Jörg; Elliott, Stephen R.; Smith, Nicholas J.; Allan, Douglas C.

doi:10.1038/s41467-022-35711-6

Title: Revealing the relationship between liquid fragility and medium-range order in silicate glasses

Journal Article · Tue Jan 03 00:00:00 UTC 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-022-35711-6 · OSTI ID:2471524

^[1];

^[2]; Zhou, Qi ^[2];

^[3]; Elliott, Stephen R. ^[4];

^[1];

^[1]

Corning Incorporated, Corning, NY (United States)
University of California, Los Angeles, CA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
University of Oxford (United Kingdom)

Despite decades of studies, the nature of the glass transition remains elusive. In particular, the sharpness of the dynamical arrest of a melt at the glass transition is captured by its fragility. Here, we reveal that fragility is governed by the medium-range order structure. Based on neutron-diffraction data for a series of aluminosilicate glasses, we propose a measurable structural parameter that features a strong inverse correlation with fragility, namely, the average medium-range distance (MRD). We use in-situ high-temperature neutron-scattering data to discuss the physical origin of this correlation. We argue that glasses exhibiting low MRD values present an excess of small network rings. Such rings are unstable and deform more readily with changes in temperature, which tends to increase fragility. These results reveal that the sharpness of the dynamical arrest experienced by a silicate glass at the glass transition is surprisingly encoded into the stability of rings in its network.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2471524

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (49)

Neutron diffraction structure factors of silicate glasses Shi, Ying; Neuefeind, Jörg; Bauchy, Mathieu Materials Data Facility https://doi.org/10.18126/2ntz-4tqe	dataset	January 2022
Effect of disorder on diffusion and viscosity in condensed systems Avramov, I.; Milchev, A. Journal of Non-Crystalline Solids, Vol. 104, Issue 2-3 https://doi.org/10.1016/0022-3093(88)90396-1	journal	September 1988
Configurational heat capacity of Na2O–CaO–Al2O3–SiO2 melts Webb, Sharon L. Chemical Geology, Vol. 256, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2008.04.003	journal	November 2008
Ring statistics analysis of topological networks: New approach and application to amorphous GeS2 and SiO2 systems Le Roux, Sébastien; Jund, Philippe Computational Materials Science, Vol. 49, Issue 1 https://doi.org/10.1016/j.commatsci.2010.04.023	journal	June 2010
Rheological and thermodynamic behaviors of different calcium aluminosilicate melts with the same non-bridging oxygen content Solvang, M.; Yue, Y. Z.; Jensen, S. L. Journal of Non-Crystalline Solids, Vol. 336, Issue 3 https://doi.org/10.1016/j.jnoncrysol.2004.02.009	journal	May 2004
Rheological and thermodynamic behavior of calcium aluminosilicate melts within the anorthite–wollastonite–gehlenite compatibility triangle Solvang, M.; Yue, Y. -Z.; Jensen, S. L. Journal of Non-Crystalline Solids, Vol. 351, Issue 6-7 https://doi.org/10.1016/j.jnoncrysol.2005.01.034	journal	March 2005
Enthalpy relaxation of hyperquenched glasses and its possible link to α- and β-relaxations Hornbøll, Lasse; Yue, Yuanzheng Journal of Non-Crystalline Solids, Vol. 354, Issue 2-9 https://doi.org/10.1016/j.jnoncrysol.2007.06.101	journal	January 2008
Compositional dependence of fragility and glass forming ability of calcium aluminosilicate melts Moesgaard, Mette; Yue, Yuanzheng Journal of Non-Crystalline Solids, Vol. 355, Issue 14-15 https://doi.org/10.1016/j.jnoncrysol.2009.04.004	journal	June 2009
Relationship between viscous dynamics and the configurational thermal expansion coefficient of glass-forming liquids Reis, Raphael M. C. V.; Mauro, John C.; Geisinger, Karen L. Journal of Non-Crystalline Solids, Vol. 358, Issue 3 https://doi.org/10.1016/j.jnoncrysol.2011.11.029	journal	February 2012
Reconciling calorimetric and kinetic fragilities of glass-forming liquids Zheng, Qiuju; Mauro, John C.; Yue, Yuanzheng Journal of Non-Crystalline Solids, Vol. 456 https://doi.org/10.1016/j.jnoncrysol.2016.11.014	journal	January 2017
Fragility and configurational heat capacity of calcium aluminosilicate glass-forming liquids Bechgaard, Tobias K.; Mauro, John C.; Bauchy, Mathieu Journal of Non-Crystalline Solids, Vol. 461 https://doi.org/10.1016/j.jnoncrysol.2017.01.033	journal	April 2017
Pressure-induced structural changes in titanophosphate glasses studied by neutron and X-ray total scattering analyses Shi, Ying; Lonnroth, Nadja T.; Youngman, Randall E. Journal of Non-Crystalline Solids, Vol. 483 https://doi.org/10.1016/j.jnoncrysol.2017.12.055	journal	March 2018
Ring size distribution in silicate glasses revealed by neutron scattering first sharp diffraction peak analysis Shi, Ying; Neuefeind, Jörg; Ma, Dong Journal of Non-Crystalline Solids, Vol. 516 https://doi.org/10.1016/j.jnoncrysol.2019.03.037	journal	July 2019
Structural evolution of fused silica below the glass-transition temperature revealed by in-situ neutron total scattering Shi, Ying; Ma, Dong; Song, Albert P. Journal of Non-Crystalline Solids, Vol. 528 https://doi.org/10.1016/j.jnoncrysol.2019.119760	journal	January 2020
The Nanoscale Ordered MAterials Diffractometer NOMAD at the Spallation Neutron Source SNS Neuefeind, Jörg; Feygenson, Mikhail; Carruth, John Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 287 https://doi.org/10.1016/j.nimb.2012.05.037	journal	September 2012
Viscous flow in simple organic liquids Laughlin, W. T.; Uhlmann, D. R. The Journal of Physical Chemistry, Vol. 76, Issue 16 https://doi.org/10.1021/j100660a023	journal	August 1972
Topological Principles of Borosilicate Glass Chemistry Smedskjaer, Morten M.; Mauro, John C.; Youngman, Randall E. The Journal of Physical Chemistry B, Vol. 115, Issue 44 https://doi.org/10.1021/jp208796b	journal	November 2011
Network Modification in Potassium Borate Glasses: Structural Studies with NMR and Raman Spectroscopies Youngman, Randall E.; Zwanziger, Josef W. The Journal of Physical Chemistry, Vol. 100, Issue 41 https://doi.org/10.1021/jp961439+	journal	January 1996
Soft colloids make strong glasses Mattsson, Johan; Wyss, Hans M.; Fernandez-Nieves, Alberto Nature, Vol. 462, Issue 7269 https://doi.org/10.1038/nature08457	journal	November 2009
Diverging views on glass transition McKenna, Gregory B. Nature Physics, Vol. 4, Issue 9 https://doi.org/10.1038/nphys1063	journal	September 2008
On the Temperature Dependence of Cooperative Relaxation Properties in Glass‐Forming Liquids Adam, Gerold; Gibbs, Julian H. The Journal of Chemical Physics, Vol. 43, Issue 1 https://doi.org/10.1063/1.1696442	journal	July 1965
Composition dependence of glass transition temperature and fragility. I. A topological model incorporating temperature-dependent constraints Gupta, Prabhat K.; Mauro, John C. The Journal of Chemical Physics, Vol. 130, Issue 9 https://doi.org/10.1063/1.3077168	journal	March 2009
Composition dependence of glass transition temperature and fragility. II. A topological model of alkali borate liquids Mauro, John C.; Gupta, Prabhat K.; Loucks, Roger J. The Journal of Chemical Physics, Vol. 130, Issue 23 https://doi.org/10.1063/1.3152432	journal	June 2009
Nonexponential relaxations in strong and fragile glass formers Böhmer, R.; Ngai, K. L.; Angell, C. A. The Journal of Chemical Physics, Vol. 99, Issue 5 https://doi.org/10.1063/1.466117	journal	September 1993
A model for phosphate glass topology considering the modifying ion sub-network Hermansen, Christian; Mauro, John C.; Yue, Yuanzheng The Journal of Chemical Physics, Vol. 140, Issue 15 https://doi.org/10.1063/1.4870764	journal	April 2014
Structural and topological aspects of borophosphate glasses and their relation to physical properties Hermansen, Christian; Youngman, Randall E.; Wang, John The Journal of Chemical Physics, Vol. 142, Issue 18 https://doi.org/10.1063/1.4919798	journal	May 2015
Atomic picture of structural relaxation in silicate glasses Song, Weiying; Li, Xin; Wang, Bu Applied Physics Letters, Vol. 114, Issue 23 https://doi.org/10.1063/1.5095529	journal	June 2019
Universal correlations between the fragility and interparticle repulsion of glass-forming liquids Lunkenheimer, Peter; Humann, Felix; Loidl, Alois The Journal of Chemical Physics, Vol. 153, Issue 12 https://doi.org/10.1063/5.0014457	journal	September 2020
Viscosity of glass-forming liquids Mauro, J. C.; Yue, Y.; Ellison, A. J. Proceedings of the National Academy of Sciences, Vol. 106, Issue 47 https://doi.org/10.1073/pnas.0911705106	journal	November 2009
Interatomic repulsion softness directly controls the fragility of supercooled metallic melts Krausser, Johannes; Samwer, Konrad H.; Zaccone, Alessio Proceedings of the National Academy of Sciences, Vol. 112, Issue 45 https://doi.org/10.1073/pnas.1503741112	journal	October 2015
Temperature-induced structural change through the glass transition of silicate glass by neutron diffraction Shi, Ying; Gulbiten, Ozgur; Neuefeind, Jörg Physical Review B, Vol. 101, Issue 13 https://doi.org/10.1103/PhysRevB.101.134106	journal	April 2020
Temperature dependence of the structures of As 2 Se 3 and As x S 1 − x glasses near the glass transition Busse, Lynda E. Physical Review B, Vol. 29, Issue 6 https://doi.org/10.1103/PhysRevB.29.3639	journal	March 1984
Structure of rings in vitreous SiO 2 Rino, José P.; Ebbsjö, Ingvar; Kalia, Rajiv K. Physical Review B, Vol. 47, Issue 6 https://doi.org/10.1103/PhysRevB.47.3053	journal	February 1993
Local elastic expansion model for viscous-flow activation energies of glass-forming molecular liquids Dyre, Jeppe C.; Olsen, Niels Boye; Christensen, Tage Physical Review B, Vol. 53, Issue 5 https://doi.org/10.1103/PhysRevB.53.2171	journal	February 1996
Universality of the high-temperature viscosity limit of silicate liquids Zheng, Qiuju; Mauro, John C.; Ellison, Adam J. Physical Review B, Vol. 83, Issue 21 https://doi.org/10.1103/PhysRevB.83.212202	journal	June 2011
Fragile-strong behavior in the As x Se 1 − x glass forming system in relation to structural dimensionality Yang, Guang; Gulbiten, Ozgur; Gueguen, Yann Physical Review B, Vol. 85, Issue 14 https://doi.org/10.1103/PhysRevB.85.144107	journal	April 2012
Role of intermediate-range order in predicting the fragility of network-forming liquids near the rigidity transition Sidebottom, D. L.; Schnell, S. E. Physical Review B, Vol. 87, Issue 5 https://doi.org/10.1103/PhysRevB.87.054202	journal	February 2013
Modified elastic model for viscosity in glass-forming systems Jaccani, Siva Priya; Gulbiten, Ozgur; Allan, Douglas C. Physical Review B, Vol. 96, Issue 22 https://doi.org/10.1103/PhysRevB.96.224201	journal	December 2017
Upper bound of fragility from spatial fluctuations of shear modulus and boson peak in glasses Novikov, V. N. Physical Review E, Vol. 106, Issue 2 https://doi.org/10.1103/PhysRevE.106.024611	journal	August 2022
Analysis of Recent Measurements of the Viscosity of Glasses Fulcher, Gordon S. Journal of the American Ceramic Society, Vol. 8, Issue 6 https://doi.org/10.1111/j.1151-2916.1925.tb16731.x	journal	June 1925
Glass Substrates for Liquid Crystal Displays Ellison, Adam; Cornejo, Iván A. International Journal of Applied Glass Science, Vol. 1, Issue 1 https://doi.org/10.1111/j.2041-1294.2010.00009.x	journal	March 2010
Microscopic Origins of Compositional Trends in Aluminosilicate Glass Properties Smedskjaer, Morten M.; Mauro, John C.; Kjeldsen, Jonas Journal of the American Ceramic Society, Vol. 96, Issue 5 https://doi.org/10.1111/jace.12298	journal	April 2013
Viscous flow of medieval cathedral glass Gulbiten, Ozgur; Mauro, John C.; Guo, Xiaoju Journal of the American Ceramic Society, Vol. 101, Issue 1 https://doi.org/10.1111/jace.15092	journal	August 2017
Predictive model for the composition dependence of glassy dynamics Guo, Xiaoju; Mauro, John C.; Allan, Douglas C. Journal of the American Ceramic Society, Vol. 101, Issue 3 https://doi.org/10.1111/jace.15272	journal	October 2017
Coarse‐grained model of the glass transition in network‐forming oxides Sidebottom, David L. Journal of the American Ceramic Society, Vol. 104, Issue 5 https://doi.org/10.1111/jace.17641	journal	January 2021
Experimental method to quantify the ring size distribution in silicate glasses and simulation validation thereof Zhou, Qi; Shi, Ying; Deng, Binghui Science Advances, Vol. 7, Issue 28 https://doi.org/10.1126/sciadv.abh1761	journal	July 2021
Formation of Glasses from Liquids and Biopolymers Angell, C. A. Science, Vol. 267, Issue 5206 https://doi.org/10.1126/science.267.5206.1924	journal	March 1995
Neutron diffraction structure factors of silicate glasses Shi, Ying; Neuefeind, Jörg; Bauchy, Mathieu Materials Data Facility https://doi.org/10.18126/2NTZ-4TQE	dataset	January 2022
Anomalous Enthalpy Relaxation in Vitreous Silica Yue, Yuanzheng Frontiers in Materials, Vol. 2 https://doi.org/10.3389/fmats.2015.00054	journal	August 2015

Similar Records

Nonlinear Acoustics at GHz Frequencies in a Viscoelastic Fragile Glass Former

Journal Article · Mon Feb 09 00:00:00 UTC 2015 · Physical Review Letters · OSTI ID:1505764

Klieber, Christoph; Gusev, Vitalyi E.; Pezeril, Thomas; +1 more

Origin of liquid fragility

Journal Article · Mon Oct 26 00:00:00 UTC 2020 · Physical Review E · OSTI ID:1706265

Ryu, Chae Woo; Egami, Takeshi

The Role of Chain Length in Nonergodicity Factor and Fragility of Polymers

Journal Article · Fri Jan 01 04:00:00 UTC 2010 · Macromolecules · OSTI ID:1015747

Sokolov, Alexei P

Related Subjects

36 MATERIALS SCIENCE
Glasses
Science & Technology
Structure of solids and liquids

Title: Revealing the relationship between liquid fragility and medium-range order in silicate glasses

Citation Formats

References (49)

Similar Records

Related Subjects