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Title: Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids

In this paper, we report the observation of a distinct correlation between the kinetic fragility index m and the reduced Arrhenius crossover temperature θA = TA/Tg in various glass-forming liquids, identifying three distinguishable groups. In particular, for 11 glass-forming metallic liquids, we universally observe a crossover in the mean diffusion coefficient from high-temperature Arrhenius to low-temperature super-Arrhenius behavior at approximately θA ≈ 2 which is in the stable liquid phases. In contrast, for fragile molecular liquids, this crossover occurs at much lower θA ≈ 1.4 and usually in their supercooled states. The θA values for strong network liquids spans a wide range higher than 2. Intriguingly, the high-temperature activation barrier E is universally found to be ~11kBTg and uncorrelated with the fragility or the reduced crossover temperature θA for metallic and molecular liquids. Finally, these observations provide a way to estimate the low-temperature glassy characteristics (Tg and m) from the high-temperature liquid quantities (E and θA).
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5]
  1. Univ. of Illinois, Urbana, IL (United States). Dept. of Nuclear, Plasma, and Radiological Engineering
  2. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Washington Univ., St. Louis, MO (United States). Dept. of Physics. Inst. of Materials Science and Engineering
  4. Univ. of Illinois, Urbana, IL (United States). Dept. of Materials Science and Engineering
  5. Univ. of Illinois, Urbana, IL (United States). Dept. of Nuclear, Plasma, and Radiological Engineering. Dept. of Materials Science and Engineering
Publication Date:
OSTI Identifier:
1337816
Grant/Contract Number:
SC0014804
Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 117; Journal Issue: 20; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Illinois, Urbana, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Orgs:
Univ. of Tennessee, Knoxville, TN (United States); Washington Univ., St. Louis, MO (United States)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE