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Abstract Glass transition is one of the unresolved critical issues in solid-state physics and materials science, during which a viscous liquid is frozen into a solid or structurally arrested state. On account of the uniform arrested mechanism, the calorimetric glass transition temperature ( T g ) always follows the same trend as the dynamical glass transition (or α -relaxation) temperature ( T α ) determined by dynamic mechanical analysis (DMA). Here, we explored the correlations between the calorimetric and dynamical glass transitions of three prototypical high-entropy metallic glasses (HEMGs) systems. We found that the HEMGs present a depressed dynamical glass transition phenomenon, i.e ., HEMGs with moderate calorimetric T g represent the highest T α and the maximum activation energy of α -relaxation. These decoupled glass transitions from thermal and mechanical measurements reveal the effect of high configurational entropy on the structure and dynamics of supercooled liquids and metallic glasses, which are associated with sluggish diffusion and decreased dynamic and spatial heterogeneities from high mixing entropy. The results have important implications in understanding the entropy effect on the structure and properties of metallic glasses for designing new materials with plenteous physical and mechanical performances.
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Collective dynamic length increases monotonically in pinned and unpinned glass forming systems
The Random First-Order Transition (RFOT) theory predicts that transport proceeds by the cooperative movement of particles in domains, whose sizes increase as a liquid is compressed above a characteristic volume fraction, ϕd. The rounded dynamical transition around ϕd, which signals a crossover to activated transport, is accompanied by a growing correlation length that is predicted to diverge at the thermodynamic glass transition density (>ϕd). Simulations and imaging experiments probed the single particle dynamics of mobile particles in response to pinning all the particles in a semi-infinite space or randomly pinning (RP) a fraction of particles in a liquid at equilibrium. The extracted dynamic length increases non-monotonically with a peak around ϕd, which not only depends on the pinning method but is also different from ϕd of the actual liquid. This finding is at variance with the results obtained using the small wavelength limit of a four-point structure factor for unpinned systems. To obtain a consistent picture of the growth of the dynamic length, one that is impervious to the use of RP, we introduce a multiparticle structure factor, Smpc(q,t), that probes collective dynamics. The collective dynamical length, calculated from the small wave vector limit of Smpc(q,t), increases monotonically as a function of the volume fraction in a glass-forming binary mixture of charged colloidal particles in both unpinned and pinned systems. This prediction, which also holds in the presence of added monovalent salt, may be validated using imaging experiments.
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- Award ID(s):
- 2320256
- PAR ID:
- 10608574
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 162
- Issue:
- 5
- ISSN:
- 0021-9606
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1063/5.0241501
