Comment on “An experimental critique on the existence of fragile-to-strong transition in glass-forming liquids”
Source abstract
Abstract
Abstract In a recent article, Zhu et al. suggest that a discrepancy exist between viscosity measurements performed by oscillation viscometry compared to other techniques such as capillary or parallel plate methods. They argue that oscillation viscometry data increasingly deviate with temperature leading to a systematic mismatch at high temperature. They conclude that this discrepancy discredit the existence of most fragile-to-strong transitions (FST) reported recently that are based on this type of measurement. Here we show that when all the data available are taken into account, this argument loses its coherency. Indeed, if FST were an artefact of instrumental error then all liquids measured using oscillation viscometry over the same temperature and viscosity range should exhibit an apparent FST. Instead, data available at high temperature for Se shows no FST but in fact show an excellent match with model prediction over the full temperature range, while data for GeSe3 measured over the same range show a severe kink revealing an FST which therefore cannot be assigned to a mismatch between measurement techniques. Furthermore we show that oscillation viscometry data can be independently corroborated using heat capacity data via the Adam Gibbs equation. Finally we show that large vapor pressure losses occur in Ge Se glasses at high temperature and are likely responsible for the reported deviation in viscosity measurement. This is not the case of oscillation viscometry measurements that are performed in sealed ampoules. Overall these results confirm the validity of oscillation viscometry as well as the existence of fragile-to-strong transitions.
Source: openaire · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Material Dynamics and Properties · Thermodynamic properties of mixtures · Phase-change materials and chalcogenides
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (25)
Show source-provided references
1. Formation of glasses from liquids and biopolymers10.1126/science.267.5206.1924 ↗
2. Thermodynamic determination of fragility in liquids and a fragile-to-strong liquid transition in water10.1038/19042 ↗
3. The influence of shear rate and temperature on the viscosity and fragility of the Zr41.2Ti13.8Cu12.5Ni10.0Be22.5 metallic-glass-forming liquid10.1016/j.actamat.2006.12.032 ↗
4. Liquid-liquid transition in a strong bulk metallic glass-forming liquid10.1038/ncomms3083 ↗
5. Fragile-to-strong transition in metallic glass-forming liquids10.1063/1.3457670 ↗
6. Structure of ZnCl2 Melt. Part II: fragile-to-strong transition in a tetrahedral liquid10.1021/acs.jpcb.7b10857 ↗
7. Phase change alloy viscosities down to Tg using Adam-Gibbs-equation fittings to excess entropy data: a fragile-to-strong transition10.1063/1.4926791 ↗
8. Structural evolution on medium-range-order during the fragile-strong transition in Ge15Te8510.1016/j.actamat.2017.02.055 ↗
9. An experimental critique on the existence of fragile-to-strong transition in glass-forming liquids10.1016/j.jnoncrysol.2018.05.009 ↗
10. Viscosity of chalcogenide melts
11. High-temperature elasticity and viscosity of GexSe1-x glasses in the transition range10.1103/PhysRevB.84.064201 ↗
12. Viscosity of selenium melt10.1016/j.jnoncrysol.2010.09.032 ↗
13. Viscosity of the glass-forming germanium-selenium liquid solutions10.1016/0022-3093(77)90124-7 ↗
14. Change in short-range order structure in selenium and tellurium melts during heating
15. Viscosity of oxygen-free vitrified systems. IV. Viscosity and structure of glasses in the selenium-germanium system
16. Doklady Akad. Nauk SSSR
17. Viscosity of glass-forming liquids10.1073/pnas.0911705106 ↗
18. Thermodynamics of structural changes in liquid Ge–Te alloys around the eutectic composition: specific heat measurements and thermodynamic stability10.1007/s00706-005-0380-1 ↗
19. A thermodynamic connection to the fragility of glass-forming liquids10.1038/35070517 ↗
20. Liquid Semiconductors
21. Industrial grade versus scientific pure: Influence on melt properties10.1063/1.5021764 ↗
22. Thermo-physical characterization of the Fe67Mo6Ni3.5Cr3.5P12C5.5B2.5 bulk metallic glass forming alloy10.1016/j.actamat.2016.07.031 ↗
23. Structural changes during a liquid-liquid transition in the deeply undercooled Zr58.5Cu15.6Ni12.8Al10.3Nb2.8 bulk metallic glass forming melt10.1103/PhysRevB.93.014201 ↗
24. Thermodynamic anomaly of the sub-Tg relaxation in hyperquenched metallic glasses10.1063/1.4803136 ↗
25. Structural evolution during fragile-to-strong transition in CuZr(Al) glass-forming liquids10.1063/1.4907374 ↗