The relaxation properties of supercooled AsxS100−x liquids are investigated using a combination of infrared photon correlation spectroscopy and topological constraint theory. Results reveal two channels of relaxation for sulfur-rich compositions that manifest by an unusual profile in the density-density autocorrelation function involving two typical timescales. This indicates a reduced temperature-dependent dynamics for one of the channels associated with a sulfur-rich segregated nanoscale phase that furthermore displays a low liquid fragility. Conversely, the dynamics of the emerging cross-linked As-S network is associated with a growth of the glass transition temperature with As content. These results can be quantitatively understood from topological constraint theory applied to a phase separated network for which a dedicated constraint enumeration must be achieved. The vanishing of this peculiar behavior occurs close to the reported isostatic reversibility window observed at the glass transition.
Complex dynamics in nanoscale phase separated supercooled liquids / Cazzato, S.; Chrissanthopoulos, A.; Micoulaut, M.; Scopigno, T.; Yannopoulos, S. N.. - In: PHYSICAL REVIEW RESEARCH. - ISSN 2643-1564. - 2:3(2020). [10.1103/physrevresearch.2.032007]
Complex dynamics in nanoscale phase separated supercooled liquids
S. Cazzato;T. Scopigno;
2020
Abstract
The relaxation properties of supercooled AsxS100−x liquids are investigated using a combination of infrared photon correlation spectroscopy and topological constraint theory. Results reveal two channels of relaxation for sulfur-rich compositions that manifest by an unusual profile in the density-density autocorrelation function involving two typical timescales. This indicates a reduced temperature-dependent dynamics for one of the channels associated with a sulfur-rich segregated nanoscale phase that furthermore displays a low liquid fragility. Conversely, the dynamics of the emerging cross-linked As-S network is associated with a growth of the glass transition temperature with As content. These results can be quantitatively understood from topological constraint theory applied to a phase separated network for which a dedicated constraint enumeration must be achieved. The vanishing of this peculiar behavior occurs close to the reported isostatic reversibility window observed at the glass transition.File | Dimensione | Formato | |
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